Favorable growth of asymmetric hetero‐nanostructures consisting of plasmonic metals and semiconductors or topological nanomaterials is highly desired because the performance of nonlinear optical antennas is closely related to their composition and morphology symmetry. In this work, two methods are proposed to overgrow PtSe2, a semiconductor or topological semimetal material, onto Au nanorods (AuNRs) to form Au/AuPt/PtSe2 and Au/AgPtSe2 heterorods via wet chemical technique. Both Au/AuPt/PtSe2 and Au/AgPtSe2 heterorods show asymmetric morphologies: the Au/AuPt/PtSe2 heterorods show a partially hollow morphology with an etched AuNR coated by AuPt and PtSe2 shells; the Au/AgPtSe2 heterorods prepared by Ag‐mediated overgrowth method have a toothbrush shape with AgPtSe2 attached on the side surface near one end of AuNRs. The two asymmetric heterorods show significantly enhanced nonlinear radiations of second harmonic generation with the excitation laser wavelength tuning from 1220 to 1315 nm, and a maximal nonlinear enhancement factor of 16 is achieved, which is attributed to the interaction of gold core with platinum selenide shell and the broken symmetry of heterostructures. The findings provide a strategy to prepare metal‐topological heterostructures as optical antennas with optimized performance in the application of nonlinear photonic nanodevices. Wet‐chemical method is applied to synthesize asymmetric heterorods through growing platinum selenide onto 1D Au nanorods. The asymmetric Au/AuPt/PtSe2 and Au/AgPtSe2 heterorods exhibit largely enhanced nonlinear emission of second harmonic generation, which is attributed to plasmonic interaction of gold core with platinum selenide shell and symmetry breaking of heterostructures.