This paper constructs a linearized transformed L1 virtual element method for the generalized nonlinear coupled time-fractional Schrödinger equations. The solutions to such problems typically exhibit singular behavior at the beginning. To avoid this pitfall, we introduce an identical s-fractional differential system derived from a smoothing transformation of variables t=s1/α, 0<α<1. By utilizing the discrete complementary convolution kernels, we prove the boundedness and error estimates of the solution of time-discrete system. Moreover, the unconditionally optimal error bounds of the proposed fully discrete scheme are derived in L2-norm without restriction on the grid ratio. Finally, numerical tests on a set of polygonal meshes are presented to verify the theoretical results.