With the integration of 5G in day-to-day devices and the foreseeable 6G revolution, demand for advanced radio frequency (RF) microelectromechanical systems (MEMS) is growing. Aluminum scandium nitride (AlScN) has emerged as the material of choice for many of those applications due to its superior piezoelectric and electromechanical properties compared to aluminum nitride (AlN). However, synthesizing high-quality, textured AlScN thin films is challenging. Alloying of Sc in AlN induces structural frustration leading to strain, defects, disoriented grains, and disrupted crystal symmetry during growth. Higher deposition temperatures, while improving crystalline quality, risk undesirable phase precipitation and limit industrial sustainability. In addition, future MEMS technologies also demand conformal and textured coatings over diverse topographies. Addressing these challenges collectively requires new and innovative synthesis approaches. In this study, we investigate the feasibility of ionized physical vapor deposition to deposit highly oriented AlScN films with minimal defects at lower temperatures. To this end, we employ combinations of different deposition approaches, such as metal-ion synchronized (MIS) high-power impulse magnetron sputtering (HiPIMS). Leveraging the high ionization rates of HiPIMS and optimally timed substrate bias potentials, we selectively bombard the growing film with Al and/or Sc ions to enhance the adatom mobility at low temperatures while simultaneously providing the ability to tune stress and coat complex structures conformally. The nonequilibrium solubility of Sc in wurtzite AlN under different conditions is investigated using a combinatorial deposition approach. Promising candidates with ∼20% Sc composition are isolated and characterized for crystallinity and residual stress. Disoriented grains, a significant issue in growing AlScN films, are observed through atomic force microscopy and found to be completely removed by substrate rotation and application of substrate biasing. The measured piezoelectric response of the films with approximately 20% Sc concentration ranges from 6.3 to 8.8 pm/V, in line with density functional theory predictions and experimentally reported values for films deposited in a production tool with coplanar geometry. At the same time, MIS-HiPIMS-deposited films offer unique properties and flexibility to tune their stress state and structural properties, thus presenting exciting opportunities for the fabrication of advanced RF filters and next-generation MEMS devices.