Single crystalline nano thin phosphor films of (Na 0.5 R 0.5 )MoO 4 :Ln 3+ (R 3+ = La, Gd), (Ln 3+ = Eu, Tb, Dy, Yb/Er) have been deposited on the quartz substrates by pulsed laser deposition (PLD) technique. In this work, we clearly explained the target preparation, pre-deposition cleaning of substrates using the piranha cleaning, and optimized growth conditions of thin films. The deposition was carried out using an 10 Nd-YAG laser (λ = 1064 nm) in an ultra-high vacuum (UHV) with an oxygen back pressure of 300 mTorr at different substrate temperature. To examine the crystal structure, 3D surface topography and film thickness, the as-deposited samples were characterized by X-ray diffraction (XRD), atomic force microscope (AFM), scanning electron microscope (SEM), respectively. The thin phosphor films possess scheelite tetragonal crystal structure with the space group I4 1 /a. The down-conversion luminescence 15 properties of Eu 3+ , Tb 3+ , Dy 3+ doped (Na 0.5 R 0.5 )MoO 4 phosphor films were studied in detail. Under 980 nm NIR laser excitation, the Yb 3+ /Er 3+ doped (Na 0.5 R 0.5 )MoO 4 thin films show intense up-converted green emission identified at 524 nm due to the transition from the populated 2 H 11/2 level to 4 I 15/2 ground level of erbium ion. The fluorescence decay time for the major transitions in (Na 0.5 R 0.5 )MoO 4 when doped with Eu 3+ ( 5 D 0 → 7 F 2 ), Tb 3+ ( 5 D 4 → 7 F 5 ), Dy 3+ ( 4 F 9/2 → 6 H 13/2 ) and Yb 3+ /Er 3+ ( 2 H 11/2 → 4 I 15/2 ) are determined and to 20 ensure the color richness, CIE color coordinates were also calculated. The obtained results suggesting that the potential (Na 0.5 R 0.5 )MoO 4 :Ln 3+ thin phosphor films can serve as an excellent material for electro/cathodo-luminescence and display applications.