The introduction of artificial illumination has brought extensive benefits to mankind, and during the last years we have seen a tremendous progress in this field with the introduction of the energy-efficient light-emitting diode (LED) and the high-contrast organic LED display. These high-end technologies are, however, produced using costly and complex processes, and it is anticipated that the next big thing in the field will be the advent of a low-cost and “green” illumination technology, which can be fabricated in a cost- and material-efficient manner using non-toxic and abundant raw materials, and which features attractive form factors such as flexibility, robustness and light-weight. The light-emitting electrochemical cell (LEC) is a newly invented illumination technology, and in this thesis we present results that imply that it can turn the above vision into reality. The thin-film LEC comprises an active material sandwiched between a cathode and an anode as its key constituent parts. With the aid of a handheld air-brush, we show that functional large-area LECs can be fabricated by simply spraying three layers of solution -- forming the anode, active material, and cathode -- on top of a substrate. We also demonstrate that such “spray-sintered” LECs can feature multicolored emission patterns, and be fabricated directly on complex-shaped surfaces, with one notable example being the realization of a light-emission fork! Almost all LECs up-to-date have been fabricated on glass substrates, but for a flexible and light-weight emissive device, it is obviously relevant to identify more appropriate substrate materials. For this end, we show that it is possible to spray-coat the entire LEC directly on conventional copy paper, and that such paper-LECs feature uniform light-emission even under heavy bending and flexing. We have further looked into the fundamental aspects of the LEC operation and demonstrated that the in-situ doping formation, which is a characteristic and heralded feature of LECs, can bring problems in the form of doping-induced self-absorption. By quantitatively analyzing this phenomenon, we provided straightforward guidelines on how future efficiency-optimized LEC devices should be designed. The in-situ doping formation process brings the important advantage that LECs can be fabricated from solely air-stabile materials, but during light emission the device needs to be protected from the ambient air. We have therefore developed a functional glass/epoxy encapsulation procedure for the attainment of LEC devices that feature a record-long ambient-air operational lifetime of 5600 h. For the light-emission device of the future, it is however critical that the encapsulation is flexible, and in our last study, we show that the use of multi-layer barrier can result in high-performance flexible LECs.