In this work, the rheological properties of the partial replacement of sodium alginate (AL) by galactomannan extracted from the seeds of L. leucocephala (GML), with or without the presence of calcium ions, were evaluated. The viscoelastic behaviour of polysaccharide blends at 15 g·L−1 showed an increase in viscosity when AL was 50% (w/w) replaced by GML. The addition of calcium ions (45 mmol) increased the apparent viscosity of the blend more than 17 times, at a shear rate of 4 s−1. Micrographs of [GML/AL/ALB] Ca2+ crosslinked particles obtained by a spraying process were analysed by AFM and revealed spherical forms with diameters in the range of 518 nm, instead of 58.4 nm in the system without albumin. The results of ALB encapsulation (97% w/w) showed that the synergistic mixture GML/AL could be used, in the future, as a new carrier system.