12Functionally graded materials (FGMs), with varying spatial, chemical and mechanical gradients 13 (continuous or stepwise), have the potential to mimic heterogenous properties found across biological 14 tissues. They can prevent stress concentrations and retain healthy cellular functions. Here, we show for 15 the first time the fabrication of polydimethylsiloxane and poly(ether) ether ketone (PDMS-PEEK) 16composites. These were successfully manufactured as a bulk material and functionally graded 17 (stepwise) without the use of hazardous solvents or the need of additives. Chemical, irreversible 18 adhesion between layers (for the FGMs) was achieved without the formation of hard, boundary 19interfaces. The mechanical properties of PDMS-PEEK FGMs are proven to be further tailorable across 20 the entirety of the build volume, mimicking the transition from soft to harder tissues. The introduction 21 of 20 wt.% PEEK particles into the PDMS matrix resulted in significant rises in the elastic modulus 22