We　report　the　proof-of-concept　of　molecularly　imprinted　polymer　(MIP)　functionalized　Bi2S3/Ti3C2TX　MXene　nanocomposites　for　photoelectrochemical　(PEC)/electrochemical　(EC)　dual-mode　sensing　of　chlorogenic　acid　(CGA).　Specifically,　the　in-situ　growth　of　the　Bi2S3/Ti3C2TX　MXene　served　as　a　transducer　substrate　for　molecularly　imprinted　polymers　such　as　PEC　and　EC　signal　generators,　due　to　its　high　surface　area,　suitable　bandwidth　and　abundant　active　sites.　In　addition,　the　chitosan　as　a　binder　was　encapsulated　into　MIP　by　means　of　phase　inversion　on　a　fluorine-doped　tin　dioxide　(FTO)　electrode.　In　the　determination　of　CGA　as　an　analytical　model,　the　dual-mode　sensor　based　on　MIP　functionalized　Bi2S3/Ti3C2TX　MXene　nanocomposites　had　good　selectivity,　excellent　stability　and　acceptable　reproducibility,　which　displayed　a　linear　concentration　range　from　0.0282　µM　to　2824　µM　for　the　PEC　signal　and　0.1412　µM　to　22.59　µM　for　the　EC　signal　with　a　low　detection　limit　of　2.4　nM　and　43.1　nM,　respectively.　Importantly,　two　dual-response　mode　with　different　transduction　mechanisms　could　mutually　conform　to　dramatically　raise　the　reliability　and　accuracy　of　detection　compared　to　single-mode　detection.　This　work　is　a　breakthrough　for　the　design　of　dual-mode　sensors　and　will　provide　a　reasonable　basis　for　the　construction　of　dual-mode　sensor　platforms.　©　2022　by　the　authors.　Licensee　MDPI,　Basel,　Switzerland.