The quasi-one-dimensional molecule-based Heisenberg antiferromagnet Cu(NO3)2(pyz)3 has an intrachain coupling J = 13.7(1) K () and exhibits a state of long-range magnetic order below TN = 0.105(1) K. The ratio of interchain to intrachain coupling is estimated to be |J'/J| = 3.3 × 10-3, demonstrating a high degree of isolation for the Cu chains.