Removal of a thin oxide layer from a tungsten ribbon and ThO₂ particulates from zircaloy surface was achieved using a pulsed Nd:YAG laser. The removal mechanism of the oxide layer from the tungsten ribbon was identified as spallation or sublimation depending on the wavelength and fluence of the coherent radiation. The oxidized and cleaned surfaces were analysed by scanning electron microscopy (SEM), energy dispersive X-ray analysis (EDS) and atomic force microscopy (AFM). Laser-cleaned tungsten ribbons were used in a thermal ionization mass spectrometer (TIMS) to determine isotopic composition of neodymium atoms. The fundamental (1064 nm) and the third harmonic (355 nm) radiations were found to be the most effective in removing ThO₂ particulates from the zircaloy surface. Decontamination efficiency was found to be critically dependent on the wavelength of the coherent radiation and number of exposures. The mechanism of cleaning of ThO₂ particulates from the zircaloy surface at different wavelengths of the incident radiation has been explained qualitatively.