A method suitable for high-resolution correlation NMR measurements on integer spin nucleus S having integer spin S and other nucleus I, different from the integer spin nucleus S and having a spin I, contained in a solid sample, said method comprising the steps of: applying an RF magnetic field having a frequency that is n times, where n is an integer equal to or greater than 2, the Larmor frequency of the integer spin nucleus S to the integer spin S; and effecting magnetization transfer between the spin I and the integer spin S, wherein said method comprises the steps of: exciting magnetization of the spin I of single quantum coherence, I (±1) where the superscript indicates the order of the coherence, by applying a first 90-degree pulse; waiting during a period of τ for converting the magnetization into heteronuclear single-quantum coherence I (±1) S between the spins I and S; applying a first overtone RF pulse and a second overtone RF pulse to the spin S with an interval of t 1 immediately after the lapse of the period of τ from the 90-degree pulse, said first and second overtone RF pulses having a frequency that is n times, where n is an integer equal to or greater than 2, the Larmor frequency of the spin S, said first overtone RF pulse serving to convert the magnetization of spin S into heteronuclear multiple quantum coherence I (±1) S (±12), and said second overtone RF pulse serving to convert the magnetization of spin S of heteronuclear multiple quantum coherence I (±1) S (±2) into magnetization I (±1) S of spin S; applying to the spin I during said period t 1 and between two periods τ a 180-degree pulse; waiting during a period of τ from the second overtone RF pulse for converting the magnetization I (±1) S of the spin S which reflects the evolution of heteronuclear multiple quantum coherence of the spin S during the period t 1 into the magnetization of the spin I of single-quantum coherence I (±1); and detecting the magnetization I (±1) of the spin I immediately after the lapse of the period of τ from the second overtone RF pulse during a period of t 2. applying an RF magnetic field having a frequency that is n times, where n is an integer equal to or greater than 2, the Larmor frequency of the integer spin nucleus S to the integer spin S; and effecting magnetization transfer between the spin I and the integer spin S, wherein said method comprises the steps of: exciting magnetization of the spin I of single quantum coherence, I (±1) where the superscript indicates the order of the coherence, by applying a first 90-degree pulse; waiting during a period of τ for converting the magnetization into heteronuclear single-quantum coherence I (±1) S between the spins I and S; applying a first overtone RF pulse and a second overtone RF pulse to the spin S with an interval of t 1 immediately after the lapse of the period of τ from the 90-degree pulse, said first and second overtone RF pulses having a frequency that is n times, where n is an integer equal to or greater than 2, the Larmor frequency of the spin S, said first overtone RF pulse serving to convert the magnetization of spin S into heteronuclear multiple quantum coherence I (±1) S (±12), and said second overtone RF pulse serving to convert the magnetization of spin S of heteronuclear multiple quantum coherence I (±1) S (±2) into magnetization I (±1) S of spin S; applying to the spin I during said period t 1 and between two periods τ a 180-degree pulse; waiting during a period of τ from the second overtone RF pulse for converting the magnetization I (±1) S of the spin S which reflects the evolution of heteronuclear multiple quantum coherence of the spin S during the period t 1 into the magnetization of the spin I of single-quantum coherence I (±1); and detecting the magnetization I (±1) of the spin I immediately after the lapse of the period of τ from the second overtone RF pulse during a period of t 2. exciting magnetization of the spin I of single quantum coherence, I (±1) where the superscript indicates the order of the coherence, by applying a first 90-degree pulse; waiting during a period of τ for converting the magnetization into heteronuclear single-quantum coherence I (±1) S between the spins I and S; applying a first overtone RF pulse and a second overtone RF pulse to the spin S with an interval of t 1 immediately after the lapse of the period of τ from the 90-degree pulse, said first and second overtone RF pulses having a frequency that is n times, where n is an integer equal to or greater than 2, the Larmor frequency of the spin S, said first overtone RF pulse serving to convert the magnetization of spin S into heteronuclear multiple quantum coherence I (±1) S (±12), and said second overtone RF pulse serving to convert the magnetization of spin S of heteronuclear multiple quantum coherence I (±1) S (±2) into magnetization I (±1) S of spin S; applying to the spin I during said period t 1 and between two periods τ a 180-degree pulse; waiting during a period of τ from the second overtone RF pulse for converting the magnetization I (±1) S of the spin S which reflects the evolution of heteronuclear multiple quantum coherence of the spin S during the period t 1 into the magnetization of the spin I of single-quantum coherence I (±1); and detecting the magnetization I (±1) of the spin I immediately after the lapse of the period of τ from the second overtone RF pulse during a period of t 2.