Magnetic properties of Ni81Fe19 (permalloy) ultrathin films with Ru and Ta capping layers (CLs) were investigated for applications to magnetic random access memory units (MRAM). The sample structure, which simulated an MRAM free layer, is Si- sub./SiO2/Ni81Fe19/Ru(Ta). The Ni81Fe19 thin films less than 3 nm thick with Ru CL show low coercive fields compared with the Ta capping layer. Both systems showed loss of momentum equivalent to magnetically dead layers of thickness (δ) ∼0.6 nm for Ru cap layer and ∼1.4 nm for Ta cap layer, respectively. Moreover, after annealing the thicknesses are slightly increased to an equivalent magnetic dead layer thickness of δ ∼ 0.84 nm and ∼1.80 nm for Ru and Ta CL, respectively. Our calculations showed that the presence of only 11% Ta concentration at the interface reduced the Ni momentum to zero, with the Ni–Ta coupling being anti-ferromagnetic; while 50% Ru intermixing at the interface reduced the Ni momentum to zero with the coupling between Ru and Ni being ferromagnetic. To find out more about the intermixing at the interface, the composition and chemical states were characterized by the x-ray photoelectron spectroscopy and peak decomposition technique. The result showed that the peak positions were different from the pure metallic case at the interface region, mainly because of the intermixing between two layers. In conclusion, the Ru capping layer might be important for MRAM use in terms of low coercive field and small δ layer thickness if compared with the Ta capping layer.