The　performance　of　photothermoelectric　materials　is　severely　limited　by　various　intrinsic　parameters　that　are　difficult　to　simultaneously　modulate,　thereby　hindering　their　applications　in　the　fields　of　photodetectors,　solar　cells,　thermoelectric　therapy　and　so　on.　In　this　study,　we　have　prepared　suspended　films　composed　of　carbon　nanotube　(CNT)　and　molybdenum　disulfide　quantum　dots　(MoS2　QDs),　which　demonstrate　a　remarkable　maximum　photothermal　conversion　efficiency　of　2201　K·mm2·W−1.　This　outstanding　performance　is　attributed　to　the　formation　of　a　heterojunction　between　CNT　and　MoS2　QDs.　Furthermore,　the　light　absorption,　temperature　coefficient　of　resistance,　and　Seebeck　coefficient　of　this　suspended　film　are　simultaneously　modulated　in　a　direction　conducive　to　enhancing　the　photothermoelectric　effect.　Consequently,　we　have　fabricated　CNT-CNT/MoS2　QDs　p-n　junction　photodetectors　to　showcase　the　improved　photoresponse　performance.　This　study　presents　an　innovative　approach　for　modulating　multiple　intrinsic　parameters　of　photothermoelectric　materials,　which　offers　valuable　insights　for　enhancing　the　performance　of　corresponding　photothermoelectric　devices.　©　2024　The　Authors