There are a range of promising applications for devices that can convert mechanical energy from their local environment into useful electrical energy. Here, mechanical energy harvesting devices have been developed to scavenge low-frequency energy from regular biomotion such as joint movement and heel strike. Specifically, these harvesters exploit novel printed nanocomposite dielectric inks in combination with commercially available conductive elastomers to develop a low cost, high performance embodiment of a variable capacitance mechanism device. The filler of the nanocomposite dielectric ink, consists of high-k dielectric nanoparticles (barium titanate and strontium doped barium titanate) functionalised with poly(methyl methacrylate) to improve the interface with the epoxy matrix. Characterisation by thermogravimetric analysis coupled to mass spectrometry and X-ray photoelectron spectroscopy confirmed the successful covalent grafting of up to ca. 16 wt% poly(methyl methacrylate) onto the dielectric nanoparticle surfaces, with a thickness of approximately 14 nm, measured by transmission electron microscopy. The dielectric inks were screen printed onto copper-polyimide foils, resulting in large area and flexible five to twenty-micron thick films with dielectric constants up to 45. Nanoparticle polymer functionalisation improved the homogeneity and stability of the inks. Using these screen-printed dielectrics with the commercial conductive elastomer, the mechanical energy harvester prototype demonstrated high mechanical cycling stability and low leakage current. It provided a promising power density of 160 μW cm−3, at low frequency (0.5 Hz), over a 1000 cycles, making the device suitable for wearable applications. This type of harvester has two advantages over the state of the art: it is mechanically flexible for integration into wearables and can be produced at low cost with printing methods.