Multiwavelength coherent light sources are key components for circuit integration of nanophotonics. Here, we demonstrated highly efficient second harmonic generation (SHG) in single-crystalline hexagonal micro-prisms (HMPs) of 3-methyl-4-methoxy-4'-nitrostilbene (MMONS) prepared via a facile self-assembled method. We found that the SHG conversion efficiency (ηSHG) of MMONS HMPs increases with increasing the prism side length (d). Local electric field |E|(2) calculations suggest that the symmetrical hexagonal prism shape of HMPs supports helically propagating modes. The SHG light produced at one end of HMP can be coupled into whispering-gallery (WG) like optical modes with a coupling efficiency of 50-80% and helically propagates along the length of HMPs toward another end. Based on this unique helical propagation of SHG light, we construct an optical interconnector by placing a single MMONS HMP on the top of a single micro-ribbon of 1,2-diphenyl-2-pyrazoline (DP). These easily fabricated MMONS HMPs can act as a coherent source, which adds a key component to the tool box of organic nano- and micro-structure optoelectronics.