The majority of modern thermal spray applications are "passive" protective coatings, but rarely performs an electronic function. However, ability to consolidate dissimilar material multilayers without substrate thermal loading has long been considered a virtue for thick-film electronics. However, complexity in understanding/controlling materials function especially due to rapidly solidification and layered assemblage has stymied expansion into electronics. The situation is changing: enhancements in process/material science are allowing reconsideration for novel electronic/sensor devices. This review critically examines past efforts in terms of materials functionality from a device perspective, along with ongoing/future concepts addressing the aforementioned deficiencies. The analysis points to intriguing future possibilities for thermal spray technology in the world of thick film sensors.