Polarity inversion is an interesting phenomenon in non-centrosymmetric wurtzite-structured aluminum nitride (AlN), which offers an important platform to establish acoustic devices with heteropolar junctions. However, previous studies showed that switching polarity generally resulted in only reversing the piezoelectric coefficient (d33) in AlN films. Here, we discovered that appropriate Cr-doping would not only allow to reverse d33 but also improve piezoelectric response in the c-axis oriented AlN films by co-sputtering dual targets of Cr and Al. Specifically, the d33 was reversed from +2.6 pC/N for the undoped AlN to −2.6 pC/N for the 6.2 at. % Cr-doped CrxAl(1−x)N films. As the Cr-doping ratio increased to 9.3 at. %, d33 was −7.0 pC/N, which was 1.7 times higher than that of the undoped AlN films. Independent PFM phase image measurement offered further evidence of the polarity inversion by comparing the undoped and 9.3 at. % Cr-doped CrxAl(1−x)N films. This work offers a simple doping strategy that allows for simultaneous reversal of piezoelectric coefficient and enhancement of piezoresponse. As a result, it establishes a promising foundation for the design and development of acoustic wave devices featuring heteropolar junctions.