Grinding processing after crushing is a common practice in mineral processing circuits involving flotation, and achieving selective liberation of target minerals by grinding is a prerequisite for successful flotation. In this study, the surface characteristics and the floatability of spodumene and feldspar particles produced by laboratory ball and short cylinder mills were determined by XRD, SEM, AFM, XPS analysis, DFT calculation, and flotation experiment. Compared with ball-milled particles, spodumene ground with short cylinder media had more exposed {110} cleavage planes, while feldspar under the same condition had more exposed {110} and {201} cleavage planes. Additionally, the amount of Al sites and the roughness of spodumene and feldspar after grinding by short cylinder media were higher than those of ball-milled particles. Micro-flotation experiments and XPS analysis further indicated that, although the co-adsorption of NaOL/DDA on the surface of spodumene is stronger than feldspar under both milling media, the flotation separation efficiency of spodumene and feldspar remained higher with short cylinder grinding media. Therefore, this study is expected to provide more reference value and theoretical guidance for the development of selective flotation separation of spodumene and feldspar from the perspective of grinding.