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The magnetic and transport properties of pulsed laser-deposited Co100−x–Cux thin films were tailored through their nano-morphology and composition by controlling for the deposition geometry, namely normal or oblique deposition, and their Cu content. All films were composed of an amorphous Co matrix and a textured growth of Cu nanocrystals, whose presence and size d increased as x increased. For x = 50, all films were superparamagnetic, regardless of deposition geometry. The normally deposited films showed no in-plane magnetic anisotropy. On the contrary, controllable in-plane uniaxial magnetic anisotropy in both direction and magnitude was generated in the obliquely deposited films. The magnetic anisotropy field Hk remained constant for x = 0, 5 and 10, Hk ≈ 35 kAm−1, and decreased to 28 and 26 kAm−1 for x = 20 and 30, respectively. This anisotropy had a magnetostatic origin due to a tilted nano-sheet morphology. In the normally deposited films, the coercive field Hc increased when x increased, from 200 (x = 0) to 1100 Am−1 (x = 30). In contrast, in obliquely deposited films, Hc decreased from 1500 (x = 0) to 100 Am−1 (x = 30) as x increased. Activation energy spectra corresponding to structural relaxation phenomena in obliquely deposited films were obtained from transport property measurements. They revealed two peaks, which also depended on their nano-morphology and composition.