In　this　study,　a　graphene　oxide　(GO)　membrane　with　tunable　interlayer　spacing　was　fabricated　by　a　facile　method　combining　the　inter-layer　modification　with　external　treatment.　Congo　red　(CR),　a　negatively　charged　dye　with　n-orbital-rich　groups,　was　adsorbed　on　nonoxide　regions　(G　regions)　of　GO　nano-sheets;　thus,　the　interlayers　were　cross-linked　by　Ca2+　ions　through　chelating　reaction.　GO@CR　nano-sheets　pi-pi　at　stacking　interactions　were　changed　by　thermal　reduction　of　the　GO/Ca/CR　membrane　using　a　hot-pressing　method.　A　broader　effective　inter-layer　spacing　control　of　the　GO　membrane　in　wet　condition　was　achieved　(from　7.7　+/-　0.2　angstrom　to　11.7　+/-　0.25　angstrom).　With　the　decrease　of　effective　inter-layer　spacing,　the　rejection　of　dyes　and　heavy　metal　ions　gradually　increased　(i.e.,　methylene　blue　(99.5%),　Cu2+　(98.6%),　Ni2+　(97.2%),　Pb2+　(97.2%)　and　Cd2+　(99.1%)　at　7.7　angstrom)　and　a　sufficient　permeation　flux　was　also　achieved　(17.1　L/m(2).h.bar).　Meanwhile,　the　diffusion　mechanism　of　water　molecules　inside　the　interlayer　gallery　of　GO　laminates　was　explored　by　climbing　image　nudged　elastic　band　(cNEB)　method.　The　hydrogen　bonding　between　water　molecules　and　hydroxyl　groups　constrained　the　diffusion　of　water　molecules;　consequently,　partially　reduced　hybrid　GO　membrane　can　show　a　better　permeability　for　water　and　superior　rejection　for　heavy　metal　ions.