Controllable patterning of bio‐compatible polymers in the presence of a cross‐linker in evaporating bi‐dispersed colloidal drops is of critical importance in functional coatings, bioprinting, and food packaging. This study investigates the effect of calcium chloride and sodium alginate concentration on the evaporative deposition and elemental distribution of dried‐out patterns. Different concentrations of alginate and salt in aqueous solutions are deposited on clean glass substrates to gain a deeper understanding of the final structures. Overall, the results indicate that changing the concentrations of sodium alginate and calcium chloride can significantly alter the elemental distribution and deposition uniformity of the final patterns. The modifications in relative concentration alter the physicochemical characteristics of the solution, resulting in significant changes in the pinning time and contact angle of the droplets that correspond to the alteration of the colloidal size and concentration, ultimately resulting in significant differences in deposition patterns. The dried‐out patterns are categorized based on their structures and mechanisms (crystallization, sedimentation, and adsorption) controlling the evaporative deposition, and then justified based on the competitive effects of cross‐linking, crystallization, and evaporation‐driven flows. Using scanning electron microscopy and energy‐dispersive X‐ray spectroscopy, the elemental distribution of dried‐out patterns is also mapped to substantiate the discussion made.