Self-assembled InAs quantum dots (QDs) in InAlAs grown on (001) and (311)B InP substrates by molecular beam epitaxy (MBE) have been comparatively investigated. A correlated study of atomic force microscopy (AFM) and photoluminescence (PL) disclosed that InAs QDs grown on high-index InP substrates can lead to high density and uniformity. By introducing a lattice-matched InAlGaAs overlayer on InAlAs buffer, still more dense and uniform InAs QDs were obtained in comparison with InAs QDs formed with only InAlAs matrix. Moreover, two-dimensional well-ordered InAs dots with regular shape grown on (311)B InP substrates are reported for the first time. We explained this exceptional phenomenon from strain energy combined with kinetics point of view.