A thermal interface material, which is obtained by bending and folding, horizontal pressing and high-temperature treatment of a laminated structure, wherein two-dimensional high-thermal-conductivity nano-sheets on the upper surface and the lower surface of the thermal interface material have a horizontal stack structure, and two-dimensional high-thermal-conductivity nano-sheets located in intermediate part between the upper surface and the lower surface of the thermal interface material have both a vertical stack structure and a curved stack structure; the thermal interface material is prepared by the following method, the method comprising the following steps: b-1) providing a laminated structure; b-2) processing the laminated structure based on modulus mismatch principle, thereby obtaining a folded laminated structure; and b-3) pressing the folded laminated structure at a first pressure in horizontal direction of the folded laminated structure, then annealing for a first time period at a first temperature, thereby obtaining the thermal interface material, wherein, the first pressure is 1.5-11 MPa, the first temperature is 2600-3100 °C; the method further comprises the following steps: c-1) providing a first slurry and a matrix which is the thermal interface material obtained in step b-3) or an intermediate part thereof, wherein the first slurry comprises a polymeric material and an optional thermal-conductivity reinforcing material; and c-2) filling or coating the matrix with the first slurry, and curing, thereby obtaining the thermal interface material. the thermal interface material is prepared by the following method, the method comprising the following steps: b-1) providing a laminated structure; b-2) processing the laminated structure based on modulus mismatch principle, thereby obtaining a folded laminated structure; and b-3) pressing the folded laminated structure at a first pressure in horizontal direction of the folded laminated structure, then annealing for a first time period at a first temperature, thereby obtaining the thermal interface material, wherein, the first pressure is 1.5-11 MPa, the first temperature is 2600-3100 °C; b-1) providing a laminated structure; b-2) processing the laminated structure based on modulus mismatch principle, thereby obtaining a folded laminated structure; and b-3) pressing the folded laminated structure at a first pressure in horizontal direction of the folded laminated structure, then annealing for a first time period at a first temperature, thereby obtaining the thermal interface material, wherein, the first pressure is 1.5-11 MPa, the first temperature is 2600-3100 °C; the method further comprises the following steps: c-1) providing a first slurry and a matrix which is the thermal interface material obtained in step b-3) or an intermediate part thereof, wherein the first slurry comprises a polymeric material and an optional thermal-conductivity reinforcing material; and c-2) filling or coating the matrix with the first slurry, and curing, thereby obtaining the thermal interface material. c-1) providing a first slurry and a matrix which is the thermal interface material obtained in step b-3) or an intermediate part thereof, wherein the first slurry comprises a polymeric material and an optional thermal-conductivity reinforcing material; and c-2) filling or coating the matrix with the first slurry, and curing, thereby obtaining the thermal interface material.