Biochar has been recognized as a promising sustainable adsorbent for removing pollutants from wastewater. In this study, two natural minerals, attapulgite (ATP) and diatomite (DE) were co-ball milled with sawdust biochar (pyrolyzed at 600 °C for 2 h) at ratios of 10-40% (w/w) and examined the ability of methylene blue (MB) to be removed from aqueous solutions by them. All the mineral-biochar composites sorbed more MB than both ball milled biochar (MBC) and ball milled mineral alone, indicating there was a positive synergy in co-ball milling biochar with these minerals. The 10% (w/w) composites of ATP:BC (MABC10%) and DE:BC (MDBC10%) had the greatest MB maximum adsorption capacities (modeled by Langmuir isotherm modeling) and were 2.7 and 2.3 times that of MBC, respectively. The adsorption capacities of MABC10% and MDBA10% were 183.0 mg g and 155.0 mg g at adsorption equilibrium, respectively. These improvements can be owing to the greater content of oxygen-containing functional groups and higher cation exchange capacity of the MABC10% and MDBC10% composites. In addition, the characterization results also reveal that pore filling, π-π stacking interactions, hydrogen bonding of hydrophilic functional groups, and electrostatic adsorption of oxygen-containing functional groups also contribute prominently to the adsorption of MB. This, along with the greater MB adsorption at higher pH and ionic strengths, suggests the roles in MB adsorption was an electrostatic interaction and an ion exchange mechanism. These results demonstrate that mineral-biochar composites prepared by co-ball milling treatment were promising sorbents of ionic contaminants for environmental applications.