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The boron phosphide (BP) semiconductor has many remarkable features, including high thermal neutron capture cross section of the 10B isotope, making it attractive for neutron detection applications. Effective and efficient neutron detection require BP to also have high crystal quality with optimum electrical properties. Here, we present the heteroepitaxial growth of high quality BP films on a superior aluminum nitride(0001)/sapphire substrate by chemical vapor deposition. The effect of process variables on crystalline and morphological properties of BP was examined in detail. BP deposited at high temperatures and high reactant flow rate ratios produced films with increased grain size and improved crystalline orientation. Narrower full width at half-maximum values of BP Raman peaks (6.1 cm–1) and ω rocking curves (352 arcsec) compared to values in the literature confirm the high crystalline quality of produced films. The films were n-type with the highest electron mobility of 37.8 cm2/V·s and lowest carrie...