Large longitudinal spin alignment of projectiles inelastically excited by Be, C, and Al targets was observed when the latter remain in their ground state. This alignment is a consequence of an angular-momentum-excitation-energy mismatch, which is well described by a DWBA cluster-model (). The longitudinal alignment of several other systems is also well described by DWBA calculations, including one where a cluster model is inappropriate, demonstrating that the alignment mechanism is a more general phenomenon. Predictions are made for inelastic excitation of for beam energies above and below the mismatch threshold.