Molybdenum　phosphide　(MoP)　is　recognized　as　one　of　the　most　promising　catalysts　for　the　hydrogen　evolution　reaction　(HER);　however　the　low　electronic　conductivity　and　complicated　synthesis　process　still　restrict　its　commercialization　as　a　replacement　for　the　benchmark　Pt/C　catalyst.　Herein,　a　novel　type　of　MoP　nanoparticles　encapsulated　with　biomolecule-derived　N,　P-codoped　carbon　nanosheets　has　been　successfully　fabricated　by　a　simple　one-step　pyrolysis　of　ammonium　molybdate　tetrahydrate,　1-hydroxyethylidene　diphosphonic　acid　(HEDP)　and　a　unique　biomolecule　guanine　as　the　precursor　of　two-dimensional　carbon　materials.　Benefiting　from　the　well-designed　architecture　with　both　good　electronic　conductivity　and　easily　accessible　catalytic　sites　provided　by　the　2D　carbon　structure,　the　optimized　catalyst　exhibits　synergistically　enhanced　HER　activity　under　both　alkaline　and　acidic　conditions,　especially　with　a　low　overpotential　of　104　mV　to　deliver　10　mA　cm-2　in　1　M　KOH.　Moreover,　the　coverage　of　N,　P-codoped　graphene-like　carbon　layers　can　prevent　the　corrosion　of　MoP　nanoparticles　in　harsh　reaction　media,　ensuring　superior　durability.　This　work　has　opened　up　a　new　direction　for　further　development　of　simple,　low-cost　but　efficient　novel　electrocatalysts.　A　one-step　pyrolysis　strategy　to　synthesize　novel　MoP　nanoparticles　encapsulated　with　biomolecule-derived　N,　P-codoped　carbon　nanosheets　for　synergistic　hydrogen　evolution　reaction.