Elemental distributions in the bulk and metal oxide surface layers of zirconium alloys play key roles in the fracture toughness of the alloys. In particular, localized hydrogen build-up leads to hydride formation and delayed hydride cracking. Parts per million levels of H in Zr have been detected using the 1.06 μm or 355 nm output of a Nd:YAG laser for ablation followed by 2+1 resonance ionization detection of H and D. Analysis of the ablation plume has shown that it consists predominately of atomic species in thermal equilibrium between 2000 and 3600°C. Ablation of thin foils has shown that the ablation rate is on the order of mono-layers per shot and increases exponentially with increasing fluence. Laser ablation depth profiling results of H distributions in an anodically grown oxide film compare qualitatively with nuclear-reaction-analysis profiling of the same sample.