We report flexible synthesis of III-Nitride nanowires and heterostructures by metal-organic chemical vapor deposition (MOCVD) via a catalytic vapor-liquid-solid (VLS) growth mechanism. Indium is used as an in-situ catalyst to facilitate and sustain the stability of liquid phase droplet for VLS growth based on thermodynamic consideration. The employment of mesoporous molecular sieves (MCM-41) helps to prevent the coalescence of catalyst droplets and to promote nucleation statistics. Cathodoluminescence (CL) of GaN nanowires shows near band-edge emission at 370nm, and strong E 2 phonon peak is observed at room temperature in Raman scattering spectra. Both binary GaN and AlN nanowires have been synthesized by MOCVD. Three-dimensional AlN/GaN trunk-branch nanostructures are reported to illustrate the versatility of incorporating the VLS mechanism into MOCVD process.