The　complementary　integration　of　perovskite　single　crystals　(PSCs)　and　silicon-based　circuitry　provides　a　feasible　way　to　combine　their　superiority　toward　efficient　multiwavelength　photodetection　and　imaging　readout;　however,　it　suffers　from　distinct　lattice　mismatch　as　well　as　the　ambiguous　coupling　interface　effect.　Herein,　we　develop　a　vacuum-assisted　vapor　deposition　strategy　to　realize　an　ultrauniform　aminosiloxane　interface-modified　silicon　wafer,　which　enables　the　monolithic　epitaxial　growth　of　PSCs　with　the　highest　mechanical　coupling　strength　up　to　340,000　N　m(-2)　achieved　so　far.　According　to　the　molecular　coupling　engineering　development　with　different　aminosiloxanes,　we　achieve　a　highly　efficient　multiwavelength-responsive　integrated　photodetector,　possessing　specific　photodetectivity　values　of　4.36　x　10(12)　jones　and　4.55　x　10(11)　jones　within　the　visible　and　NIR　regions,　respectively,　as　well　as　the　lowest　X-ray　detection　limit　of　42.6　nGy(air)　s(-1).　Moreover,　a　particularly　wide　-3dB　cut-off　frequency　of　6350　Hz　as　well　as　a　120　dB　linear　dynamic　range　(LDR)　also　endows　the　integrated　device　with　excellent　dynamic　photodetection　capability.　This　work　provides　an　efficacious　approach　in　the　integration　technology　for　PSC-based　optoelectronic　applications.