The　2D　ternary　transition　metal　phosphorous　chalcogenides　(TMPCs)　have　attracted　extensive　research　interest　due　to　their　widely　tunable　band　gap,　rich　electronic　properties,　inherent　magnetic　and　ferroelectric　properties.　However,　the　synthesis　of　TMPCs　via　chemical　vapor　deposition　(CVD)　is　still　challenging　since　it　is　difficult　to　control　reactions　among　multi-precursors.　Here,　a　subtractive　element　growth　mechanism　is　proposed　to　controllably　synthesize　the　TMPCs.　Based　on　the　growth　mechanism,　the　TMPCs　including　FePS3,　FePSe3,　MnPS3,　MnPSe3,　CdPS3,　CdPSe3,　In2P3S9,　and　SnPS3　are　achieved　successfully　and　further　confirmed　by　Raman,　second-harmonic　generation　(SHG),　and　scanning　transmission　electron　microscopy　(STEM).　The　typical　TMPCs-SnPS3　shows　a　strong　SHG　signal　at　1064　nm,　with　an　effective　nonlinear　susceptibility　chi(2)　of　8.41　x　10-11　m　V-1,　which　is　about　8　times　of　that　in　MoS2.　And　the　photodetector　based　on　CdPSe3　exhibits　superior　detection　performances　with　responsivity　of　582　mA　W-1,　high　detectivity　of　3.19　x　1011　Jones,　and　fast　rise　time　of　611　mu　s,　which　is　better　than　most　previously　reported　TMPCs-based　photodetectors.　These　results　demonstrate　the　high　quality　of　TMPCs　and　promote　the　exploration　of　the　optical　properties　of　2D　TMPCs　for　their　applications　in　optoelectronics.　The　controllable　synthesis　of　transition　metal　phosphorous　chalcogenides　(TMPCs)　based　on　subtracting　elements　mechanism　is　reported.　Among　them,　the　SnPS3　exhibits　effective　nonlinear　susceptibility　chi(2)　of　8.41　x　10-11　m　V-1.　The　CdPSe3　photodetector　displays　high　responsivity　(582　mA　W-1)　and　detectivity　(3.19　x　1011　Jones).　This　research　will　pave　the　way　for　exploration　of　ternary　TMPCs　in　optical　and　photoelectric　detection.image