A method of preparing a surface functionalized porous organic-inorganic hybrid material comprising: (a) performing a pre-treatment process of removing water or a solvent bonded to the coordinatively unsaturated metal sites of a porous organic-inorganic hybrid material; (b) reacting the porous organic-inorganic hybrid material having unsaturated metal sites with an organic substance selected from among compounds represented by Formulas 1 to 3 below: H 2 N-M-R 1 (Formula 1) HS-M-R 2 (Formula 2) 2 OP-M-R 3 (Formula 3) wherein M is an alkylene or aralkylene group of C 1 - C 20 including or not including unsaturated hydrocarbons, and each of R 1, R 2 and R 3 is independently an organic alkylene or aralkylene group, substituted with one or more selected from among halogen elements, a vinyl group (-C=CH 2), an amino group (-NH 2), an imino group (-NHR 14), a mercapto group (-SH), a hydroxyl group (-OH), a carboxylic acid group (-COOH), a sulfonic acid group (-SO 3 H), an alkoxy group (-OR) and a phosphoric group (-PO 2) or an inorganic substance selected from among polyoxometallate of [AlO 4 Al 12 24 (H 2 O) 12] 7+ or [PW 12 O 40] 3- wherein the organic substance or the inorganic substance is bonded to the coordinatively unsaturated metal sites of the surface functionalized porous organic-inorganic hybrid material; wherein the porous organic-inorganic hybrid material is a crystalline polymer compound formed by bonding an organic ligand with a central metal ion and has a molecule-sized pore structure or a nano-sized pore structure; and wherein the precursor of the central metal ion of the porous organic-inorganic hybrid material is one or more metals selected from among Ti, Zr, Hf, V, Nb, Ta, Cr, Mo, W, Mn, Re, Fe, Ru, Os, Co, Rh, Ir, Ni, Pd, Pt, Cu, Ag, Au, Zn, Cd, Hg, Mg, Ca, Sr, Ba, Sc, Y, Al, Ga, In, Tl, Si, Ge, Sn, Pb, As, Sb and Bi, or metal compounds thereof. (a) performing a pre-treatment process of removing water or a solvent bonded to the coordinatively unsaturated metal sites of a porous organic-inorganic hybrid material; (b) reacting the porous organic-inorganic hybrid material having unsaturated metal sites with an organic substance selected from among compounds represented by Formulas 1 to 3 below: H 2 N-M-R 1 (Formula 1) HS-M-R 2 (Formula 2) 2 OP-M-R 3 (Formula 3) wherein M is an alkylene or aralkylene group of C 1 - C 20 including or not including unsaturated hydrocarbons, and each of R 1, R 2 and R 3 is independently an organic alkylene or aralkylene group, substituted with one or more selected from among halogen elements, a vinyl group (-C=CH 2), an amino group (-NH 2), an imino group (-NHR 14), a mercapto group (-SH), a hydroxyl group (-OH), a carboxylic acid group (-COOH), a sulfonic acid group (-SO 3 H), an alkoxy group (-OR) and a phosphoric group (-PO 2) or an inorganic substance selected from among polyoxometallate of [AlO 4 Al 12 24 (H 2 O) 12] 7+ or [PW 12 O 40] 3- an organic substance selected from among compounds represented by Formulas 1 to 3 below: H 2 N-M-R 1 (Formula 1) HS-M-R 2 (Formula 2) 2 OP-M-R 3 (Formula 3) wherein M is an alkylene or aralkylene group of C 1 - C 20 including or not including unsaturated hydrocarbons, and each of R 1, R 2 and R 3 is independently an organic alkylene or aralkylene group, substituted with one or more selected from among halogen elements, a vinyl group (-C=CH 2), an amino group (-NH 2), an imino group (-NHR 14), a mercapto group (-SH), a hydroxyl group (-OH), a carboxylic acid group (-COOH), a sulfonic acid group (-SO 3 H), an alkoxy group (-OR) and a phosphoric group (-PO 2) or an inorganic substance selected from among polyoxometallate of [AlO 4 Al 12 24 (H 2 O) 12] 7+ or [PW 12 O 40] 3-