We present an innovative approach to integrate arrays of isolated, strain-free GaN crystals on patterned Si substrates. First, micrometer-sized pillars are patterned onto Si(0 0 1) substrates. Subsequently, 2.5 μm Si substrates are deposited by low-energy plasma-enhanced chemical vapor deposition, forming crystals mostly bounded by {1 1 1}, {1 1 3}, and {15 3 23} facets. Plasma-assisted molecular beam epitaxy is then used for GaN deposition. GaN crystals with slanted {0 0 0 1} facets having a root-mean-square surface roughness of 0.7 nm are obtained for a deposited material thickness of >3 μm. Microphotoluminescence measurements performed at room and cryogenic temperature show no yellow luminescence and a neutral donor-bound A exciton transition at 3.471 eV (10 K) with a full width at half-maximum of 10 meV. Microphotoluminescence and micro-Raman spectra reveal that GaN grown on Si pillars is …