Our previous studies on AlN microstructures have shown that smooth amorphous films (a-AlN) can be grown on negatively biased Si substrates by the versatile physical vapour deposition technique under reactive magnetron sputtering. These a-AlN films are produced by energetic Ar ion bombardment under negative bias whereas those grown without bias were columnar crystallized ones (c-AlN). Here, we show first that depositing an a-AlN layer on c-AlN/Si structures by switching a suitable bias to the Si substrate can efficiently reduce their surface roughness. We then extend this smoothening method to a c-AlN/Poly-crystallized diamond (PCD) structure to reduce its high surface roughness that hampers using such structures in SAW device design. In fact, the piezoelectric c-AlN surfaces grown on rough diamond surfaces are equally rough. Effectively, the a-AlN layer deposited on the c-AlN/PCD structure brings down the latter's RMS surface roughness to one tenth of its initial RMS roughness, as confirmed here by TEM and AFM observations. The insulating property of the diamond as biased substrate doesn't impede the growth of this a-AlN layer. This smoothening method is without process interruption, where simply a negative bias is switched on to the diamond substrate once the desired piezoelectric c-AlN film thickness as monitored here by in-situ reflectometry, is attained. This as-grown smoothening method can be therefore easily and rapidly implemented and can thus replace time-consuming and costly PCD ionic and/or mechanical polishing. Hopefully, the method can be advantageously applied to c-AlN/nano-crystallized diamond structures (NCD) where the NCD films are not prepared under rigorous conditions meant to minimize their surface roughness.