The formation of single-crystalline configurations by the oriented attachment of calcite was experimentally demonstrated as 3D bundles in a nonaqueous system. In the initial stage, 1D short chains elongated in the c direction were formed through the primary oriented attachment of calcite nanoblocks similar to 30 nm in diameter. The 3D bundles were then produced through subsequent side-by-side oriented attachment of the 1D chains in the progressive stage. Finally, micrometer-sized single-crystalline architectures were constructed via large-scale oriented attachment of the nanoscale building blocks with a decrease in repulsion force due to the surface charge.