Unique　nanofoams　consisting　of　interweaved　ultrathin　graphene　confining　Zn–N–C　dipoles　(ZnNG)　are　constructed　via　calcination　of　Zn-coordinated　precursor.　Due　to　the　introduction　of　local　polar　Zn–N–C　configurations,　with　hypersensitivity　for　mechanical　stress,　the　piezoelectricity　is　created　on　the　nonpiezoelectric　graphene,　and　the　hierarchical　ZnNG　exhibits　obvious　piezocatalytic　activity　of　water　splitting　for　H2　production　even　under　mild　agitation.　The　corresponding　rate　of　H2　production　is　about　14.65　μmol　g−1　h−1.　It　triggers　a　breakthrough　in　piezocatalytic　H2　evolution　under　low-frequency　vibration,　and　takes　a　significant　step　forward　for　piezocatalysis　towards　practical　applications.　Furthermore,　the　presented　concept　of　confining　atomic　polar　configuration　for　engineering　piezoelectricity　would　open　up　new　horizon　for　constructing　new-type　piezoelectrics　based　on　both　piezoelectric　and　nonpiezoelectric　materials.　©　2022　Science　Press　and　Dalian　Institute　of　Chemical　Physics,　Chinese　Academy　of　Sciences.　Published　by　ELSEVIER　B.V.　and　Science　Press.