Employing　a　rational　design　strategy　to　construct　porous　metal　organic　frameworks　(MOFs)　with　predictable　structures　for　specific　applications　still　remains　one　of　the　most　compelling　challenges.　Here,　a　novel　two-dimensional　(2D)　bilayer　(FJI-H16)　based　on　Zn/Cd　heterometal　clusters　has　been　constructed　throughout　a　heterometal　strategy,　further　introducing　pillar　ligands　with　different　sizes　and　flexibilities　that　expand　such　2D　bilayer　structures　into　two　novel　three-dimensional　(3D)　frameworks　(FJI-H17,　FJI-H18),　in　which　both　the　pore　size　and　flexibility　of　the　new-formed　3D　frameworks　can　be　tuned.　Further　gas　adsorption　research　indicates　that　the　less　porous　FJI-H16　has　the　highest　H-2　adsorption,　while　the　very　porous　FJI-H17　has　the　highest　CO2　adsorption.　The　relationship　between　gas　adsorption　properties　and　pore　characteristics　also　has　been　investigated,　which　will　provide　a　potential　strategy　that　can　improve　gas　adsorption　in　designing　porous　MOFs.