The efficiency of the recently proposed iCIPT2 [iterative configuration interaction (iCI) with selection and second-order perturbation theory (PT2); J. Chem. Theory Comput. 2020, 16, 2296] for strongly correlated electrons is further enhanced (by up to 20×) by using (1) a new ranking criterion for configuration selection, (2) a new particle-hole algorithm for Hamiltonian construction over randomly selected configuration state functions (CSF), and (3) a new data structure for the quick sorting of the variational and first-order interaction spaces. Meanwhile, the memory requirement is also significantly reduced. As a result, this improved implementation of iCIPT2 can handle 1 order of magnitude more CSFs than the previous version, as revealed by taking the chromium dimer and an iron–sulfur cluster, [Fe₂S₂(SCH₃)]₄^2–, as examples.