Thin film flexible electronics refer to a class of electronic devices manufactured by multiple layering and scribing on flexible polymer substrates. Examples of such devices includes printed Li batteries, flexible photovoltaic cells and light emitting diodes. These devices are often mass manufactured by Roll-to-Roll processing (R2R). Whilst the basic technology is well established, the increasing demands on precision environmental protection and multi layering of devices means that in-process measurement of printed surface features is a critical bottle neck in terms of developing R2R as a process route. The purpose of the present paper is to review the current critical dimensional metrology needs in R2R manufacture and in particular to highlight the development of a new in-process surface metrology system based on Multi-wavelength Polarizing Interferometry (MPI). The system is capable of measurement in real time, is environmentally robust and has nanometre resolution. The paper concludes by highlighting an example of the first trial implementation of the MPI on a production level R2R machine and discussed issues with quantification of film dimensions and associated signal processing.