Polydimethylsiloxane (PDMS) is widely used for bio-medical, optical and microfluidic applications. Hence, PDMS layers on free-form surfaces on defined areas are needed. Conventional ways such as spin coating show drawbacks by long processing time and no sufficient application on free form surfaces. In this work, laser direct writing with UV-curable PDMS on a curved surface was performed. The coating technique using aerosol jet printing showed thin film thicknesses, compared to conventional spin coating techniques, obtaining controllable layer thickness down to 3.5 µm in 5 min on an area of 600 mm2 and on non-flat surfaces. Deposition rate control achieved layer thicknesses between 3.5 and 25.7 µm. The combination of material deposition and x–y galvanometric mirror scanner-based laser direct writing leads to a hybrid approach aiming for several applications in the fields of surface functionalization, and bio-medical and sensory applications. In addition, the procedure is able to overcome the batch-based PDMS processing and introduce the continuous flow-based application.