The functionalisation of low-cost steel over large areas with low cost intermediate layers (ILs) for utilisation as substrates in thin film solar modules is reported. Three approaches for the deposition of ILs are demonstrated and evaluated; a thick SiOx sol–gel based on a one-step acidic catalysis applied by spray technique, a commercial screen-printable dielectric ink, and an epoxy-based material (SU8) deposited by screen printing or bar coating. These ILs demonstrated the properties of surface levelling (quantified by mechanical profilometry), electric insulation (tested using breakdown voltage and leakage current) and acted as an anti-diffusion barrier (demonstrated with glow discharge mass spectrometry). Moreover, the performances of amorphous silicon (a-Si:H) and organic photovoltaic (OPV) thin film solar cells grown on carbon and stainless steels (a-Si:H: 5.53% and OPV: 2.40%) show similar performances as those obtained using a reference glass substrate (a-Si:H: 5.51% and OPV: 2.90%). Finally, a cost analysis taking into account both the SiOx sol–gel and the dielectric ink IL was reported to demonstrate the economic feasibility of the steel/IL prototypes.