Development　of　high-efficiency　and　low-cost　electrocatalyst　for　oxygen　evolution　reaction　(OER)　is　very　important　for　use　at　alkaline　water　electrolysis.　Metal-organic　frameworks　(MOF)　provide　a　rich　platform　for　designing　multi-functional　materials　due　to　their　controllable　composition　and　ultra-high　surface　area.　Herein,　we　report　our　findings　in　the　development　of　amorphous　nickel–cobalt　bimetal-organic　framework　nanosheets　with　crystalline　motifs　via　a　simple　＇ligands　hybridization　engineering＇　strategy.　These　complexes’　ligands　contain　inorganic　ligands　(H2O　and　NO3−)　and　organic　ones,　hexamethylenetetramine　(HMT).　Further,　we　investigated　a　series　of　mixed-metal　with　multi-ligands　materials　as　OER　catalysts　to　explore　their　possible　advantages　and　features.　It　is　found　that　the　Ni　doping　is　an　effective　approach　for　optimizing　the　electronic　configuration,　changing　lattice　ordering　degree,　and　thus　enhancing　activities　of　HMT-based　electrocatalysts.　Also,　the　crystalline-amorphous　boundaries　of　various　HMT-based　electrocatalyst　can　be　easily　controlled　by　simply　changing　amounts　of　Ni-precursor　added.　As　a　result,　the　optimized　ultrathin　(Co,　0.3Ni)-HMT　nanosheets　can　reach　a　current　density　of　10　mA　cm−2　at　low　overpotential　of　330　mV　with　a　small　Tafel　slope　of　66　mV　dec−1.　Our　findings　show　that　the　electronic　structure　changes　induced　by　Ni　doping,　2D　nanosheet　structure,　and　MOF　frameworks　with　multi-ligands　compositions　play　critical　roles　in　the　enhancement　of　the　kinetically　sluggish　electrocatalytic　OER.　The　present　study　emphasizes　the　importance　of　ligands　and　active　metals　via　hybridization　for　exploring　novel　efficient　electrocatalysts.　©　2020　Science　Press