Transport and magnetic properties of La_0.67Sr_0.33MnO₃ (LSMO) manganite thin films and bicrystal junctions were investigated. Epitaxial manganite films were grown on SrTiO₃, LaAlO₃, NdGaO₃ (NGO), and (LaAlO₃)_0.3 + (Sr₂AlTaO₆)_0.7 substrates, and their magnetic anisotropy were determined by two independent techniques of magnetic resonance spectroscopy. It was demonstrated that by using these techniques, a small (0.3%) anisotropy of crystal structure at the (110) surface plane of the orthorhombic NGO substrate leads to uniaxial magnetic anisotropy of the films in the plane of the substrate at least at the room temperature. It was found that on vicinal NGO substrates, the value of magnetic anisotropy strength can be varied in the range 100–200 Oe at T = 295 K by changing the substrate vicinal angle from 0° to 25°. Measurement of the magnetic anisotropy of manganite bicrystal junction demonstrated the presence of two ferromagnetic spin subsystems for both types of bicrystal boundaries with tilting of basal plane of manganite tilted bicrystal (TB-junction) and with rotation of crystallographic axes (RB-junction) used for comparison. The magnetoresistance of TB-junctions increases with decreasing temperature and the misorientation angle. Variation of bicrystal misorientation angle does not lead to change of misorientation of easy magnetic axes in the film parts forming TB-junction. Analysis of the voltage dependencies of bicrystal junction conductivity show that the low value of the magnetoresistance for the LSMO bicrystal junctions can be caused by two scattering mechanisms. The first one is the spin-flip of spin-polarized carriers due to the strong electron-electron interactions in a disordered layer at the bicrystal boundary at low temperatures and the second one is spin-flip by antiferromagnetic magnons at high temperatures.