[Zn 2 (Oxac)(Taz) 2 ]¢(H 2 O) x , referred to as ZOTW x , was prepared from aqueous methanol solutions of Zn 5 (CO 3 ) 2 (OH) 6 and two kinds of ligands, 1,2,4-triazole (Taz) and oxalic acid (Oxac), at 453 K under magnetic fields of up to 6 T. The magnetic fields markedly changed the morphology from irregular agglomerates at zero field to rectangular-prism crystals having smooth surfaces at 6 T, although the monoclinic crystal structure was only slightly deformed to a triclinic one. As-synthesized ZOTW x (H) prepared under magnetic fields of H/T ² 2 adsorbed a large amount of N 2 at 77 K in rectangular Type I adsorption isotherms even without the usual pretreatment at 383 K and 1 mPa. It suggests that high magnetic fields induced the formation of hydrophobic micropores having uniform sizes. The hydrophobicity was consistent with the results that the water-assisted micropore formation was depressed in the as-synthesized ZOTW x (H) containing a small amount of water. Porous coordination polymers (PCPs) are a new class of porous crystalline materials that have extremely high porosity and selective adsorptivity for guest molecules.112 Gas storage capacity in PCPs was promoted by introducing open metal sites, 6 increasing the surface area, 7 and modifying pores with functionalized organic linker.8 The gate-controlled adsorption was found that the latent pores of flexible PCPs opened above a critical pressure.4,9 Such flexible PCPs were brought about after desolvation. The amounts of solvent surrounded by the frameworks of PCPs are very important for the formation of latent pores and their flexibility, as well as pore volume and adsorptivity.We found a new route for micropore formation of one of the PCPs, [Zn 2 (Oxac)(Taz) 2 ]¢(H 2 O) 2.5 referred to as ZOTW 2.5 ; i.e., the micropore formation via water-assisted CO 2 adsorption on ZOTW x .13 Although the as-synthesized ZOTW 2.5 pretreated gently had little open micropores because of some residual water, the water-assisted adsorption of CO 2 to bring about the formation of abundant open micropores after vacuum degassing.Magnetic fields (H/T) drastically modify the structures and properties of materials, especially colloidal systems.1419 Homogeneous magnetic fields affect them thermodynamically via magnetic energy, (1/2)»H 2 , which may induce magnetic orientation, phase transition, etc. The magnetic field gradient also brings about a magnetic force, which causes convection, mass-transport, concentration change, etc. In this study, magnetic field control of the pore formation of a PCP comprising metal ions and magnetically anisotropic ligands was investigated. ZOTW 2.5 was synthesized under magnetic fields of up to 6 T, and the morphology of the crystals, crystal structure, size, and properties of the micropores were examined. The experiments have been described in a previous paper. 13 0.4 g of Zn 5 (CO 3 ) 2 (OH) 6 , 0.4 g of H 2 C 2 O 4 , and 1.4 g of 1,2,4-triazole were added to a mixed solvent of 12 mL of methanol and 2 mL of distilled water. The dispersion was tran...