The effects of cesium (Cs) ion-implantation on uncured plasma-enhanced chemical-vapor-deposited organosilicate low dielectric constant (low-k) (SiCOH) films have been investigated and compared with an ultraviolet (UV) cured film. The mechanical properties, including the elastic modulus and hardness, of the SiCOH low-k films are improved by up to 30% with Cs implantation, and further up to 52% after annealing at 400 °C in a N2 ambient for 1 h. These improvements are either comparable to or better than the effects of UV-curing. They are attributed to an enhancement of the Si-O-Si network structure. The k-value of the SiCOH films increased slightly after Cs implantation, and increased further after annealing. These increases are attributed to two carbon-loss mechanisms, i.e., the carbon loss due to Si-CH3 bond breakage from implanted Cs ions, and the carbon loss due to oxidation during the annealing. The time-zero dielectric breakdown strength was improved after the Cs implantation and the annealing, and was better than the UV-cured sample. These results indicate that Cs ion implantation could be a supplement to or a substitution for the currently used UV curing method for processing SiCOH low-k films.