Phenylurea　has　been　integrated　into　the　traditional　polymerization　route　of　carbon　nitride　(CN)　precursors　(e.g.,　urea,　thiourea,　dicyandiamide,　and　ammonium　thiocyanide)　in　a　facile　one-pot　approach,　to　modify　the　chemical　composition,　electronic　structure,　and　catalytic　performance　of　graphitic　CN　(g-CN).　Results　revealed　that　the　co-polymerization　of　phenylurea　with　urea　dramatically　modifies　the　optical　and　electronic　properties　of　g-CN,　leading　to　a　remarkable　improvement　by　a　factor　of　9　in　the　photocatalytic　activity　of　g-CN　(when　coupled　with　Pt　as　a　co-catalyst)　in　an　assay　of　hydrogen　evolution　reaction,　while　still　keeping　a　high　catalytic　stability　during　pre-longed　operations.　The　active　catalyst　is　eventually　a　hybrid　organocatalyst　that　is　a　heterogeneous　Pt　catalyst　supported　on　a　urea-based　polymer.　The　promotional　effect　of　phenylurea　as　the　co-monomer　for　urea　on　the　activity　and　stability　of　Pt/g-CN　could　be　related　to　the　extension　of　delocalized　π-conjugated　system　of　CN　heterocycles,　as　a　result　of　the　fusion　of　phenyl　motifs　in　the　CN　framework.　The　thus　created　surface　dyadic　structure　favors　the　separation　and　migration　of　charge-carriers　photoexcited　upon　light　illumination.　This　work　highlights　a　wide　accessibility　of　chemical　protocols　for　the　design　and　synthesis　of　functional　CN　photocatalysts　at　molecular　levels　by　applying　suitable　CN　precursors　and　co-monomers.　©　2013　Elsevier　Inc.　All　rights　reserved.