Flexible electronics are anticipated to be one of the next technological advancements of electronic devices. The enhanced durability, light-weight nature, and conformity of flexible electronics are desired properties in a variety of fields and are anticipated to reduce production costs. Two promising materials for use in flexible electronics are carbon nanotube (CNT) films and laser-crystallized thin silicon films. CNTs are in their infancy in respect to their presence in electronic devices; however their superb mechanical and electronic properties make them ideal candidates for flexible electronics. Thin silicon films are a natural transition from bulk silicon as bulk silicon has been the preferred material in electronics since the dawn of the transistor. Thin-film silicon retains the well-studied electronic properties of bulk silicon; however, it becomes flexible as it is thinned. Obstacles to the application of both these materials in flexible electronics nonetheless exist. Compressed CNT films undergo strain softening – a mechanism in which the CNT film restructures itself in response to an applied strain, which reduces the Young’s modulus and electronic conductivity. In this dissertation, thin CNT films are capped with a thin polymer layer, with the aim to mitigate strain softening through excluded volume interactions in a bilayer format that serves as a paradigm for more sophisticated device relevant settings. More specifically, metallic and semiconducting CNT films of different thicknesses are capped with a polystyrene film of comparable thickness, and the mechanical and electronic strain response of the capped CNT film is examined and discussed. Ultrathin silicon films cannot be grown as monocrystalline silicon, so amorphous silicon films must be deposited and crystallized. Laser crystallization is an alternative to oven annealing and has a faster throughput. In this dissertation, amorphous silicon films of various thicknesses were deposited on several substrates via plasma enhanced chemical vapor deposition. The films were crystallized with a pulsed Nd:YVO4 laser operating at the third harmonic of 355 nm, and the structural and electronic properties were characterized to determine the effects of film thickness and substrate composition.