Assembly　of　two-dimensional　(2D)　layered　structures　into　three-dimensional　(3D)　macroscopic　hydrogel　has　been　an　enduring　attracting　research　theme.　However,　the　anisotropic　intersheet　cross-linking　to　form　Ti3C2Tx　MXene-based　hydrogel　remains　intrinsically　challenging　because　of　the　superior　hydrophilic　nature　of　2D　Ti3C2Tx.　Herein,　Ti3C2Tx　MXene　is　ingeniously　assembled　into　the　3D　macroscopic　hydrogel　under　mild　conditions　by　a　graphene　oxide　(GO)-assisted　self-convergence　process.　During　the　process,　GO　is　reduced　to　reduced　graphene　oxide　(RGO)　by　virtue　of　the　reduction　ability　of　Ti3C2Tx,　leading　to　the　partial　removal　of　hydrophilic　oxygen-containing　groups　and　an　increase　of　the　hydrophobicity　and　the　π-conjugated　structures　of　RGO,　which　enables　the　assembly　of　RGO　into　a　3D　RGO　framework.　Simultaneously,　Ti3C2Tx　is　self-converged　to　be　incorporated　into　the　RGO　framework　by　intimate　interfacial　interactions,　thereby　generating　Ti3C2Tx-based　hydrogel.　The　hydrogel　with　interconnected　porous　structure　holds　great　potential　as　a　promising　material　platform　for　photoredox　catalysis.　With　the　incorporation　of　Eosin　Y　photosensitizer,　the　functional　Ti3C2Tx-based　hydrogel　exhibits　enhanced　photoactivity　compared　to　the　powder　counterpart　and　features　easy　operability.　This　work　enriches　the　rational　utilization　of　GO/MXene　colloid　chemistry　to　design　Ti3C2Tx　MXene-based　hydrogels　with　improved　overall　efficacy　in　practical　applications.　©　2018　American　Chemical　Society.