Batch experiments were performed to study metal sorption by pine bark and algae-treated bark. The biosorption of copper (Cu), lead (Pb), zinc (Zn), cadmium (Cd), cobalt (Co), and nickel (Ni) in synthetic multimetal aqueous solutions was studied as a function of metal content in solution, and amount and size of bark particles used for sorption. Influence of water hardness (Ca2+ only was tested) on the metal sorption process was also evaluated. Metal uptake from solutions with high heavy metal content (i.e. 10× the limit for leachate from landfills) was found to be independent of Ca2+ concentration. At low metal content in solution (i.e. 1× the limit for leachate from landfills), uptake of Cu, Zn, Ni, and Cd decreased with increasing Ca2+ content in water. Microalgae-treated bark was found to increase the metal sorption efficiency. Air-drying of bark-entrapped algae was shown to be the best method for sorbent drying. In general, the green algae, Chlorella sp. and Pseudokirchneriella subcapitata showed the best results in metal uptake. Sorption of Co, Zn, Ni, and Cd from solution with high levels of both heavy metals and calcium increased by almost 50% with algae treatment of bark was applied. At low levels of metals and calcium content, 100% uptake of Cu and Pb in water was observed. Uptake of other metals from solution with low metal and Ca content was relatively high (50–60%). Low pH (pH 3.0) had no influence on metal sorption from solutions with high metal content. For solutions with low metal content a decrease of metal uptake by 10–15% was observed for all the metals but Pb. Thus, the treatment of bark with microalgae was successful and influenced positively the uptake capacity of the bark.