Provided are compositions that include a nematic colloid, the nematic colloid comprising a nematic liquid crystal and a key colloid; and a lock colloid, the lock colloid optionally having at least two arms extending therefrom, the lock colloid being configured for assembly with the key colloid of the nematic colloid, the assembly optionally being mediated by a dipole interaction between the colloid and the lock colloid, by a disinclination line of the nematic colloid, or any combination thereof. Also provided are related methods. The disclosed compositions and methods can be used to, e.g., assemble chain and lattice structures from the key colloids by exploiting disinclination lines and dipole defects of the components of the compositions.