To meet the rising data-offloading demands, IEEE 802.11-based WiFi networks have undergone consistent densification. The unlicensed spectrum has also been harnessed through LTE-WiFi coexistence. However, in dense and ultradense networks (DNs/UDNs), the network capacity is even more adversely impacted by the endemic interference. Yet, the precise nature of Capacity Interference Relationship (CIR) in DNs/UDNs and LTE-WiFi coexistence remains to be studied. Densification also exacerbates the challenges to network optimization. The conventional approaches to simplify the complex SINR-Capacity constraints lead to high convergence times in DN/UDN optimization. We investigate the CIR in dense and ultra-dense WiFi (IEEE 802. 11a) and LTE-WiFi (LTULAA) networks through real-time experiments. We then subject the empirical data to linear and polynomial regression to determine the nature of CIR and demonstrate that strong linear correlations may exist. We also study the impact of predictor variables, topology, and radio access technology on CIR. Most importantly, we propose CIRNO, a CIR-inspired network optimization approach, wherein the empirically determined CIR equation replaces the theoretically assumed SINR-Capacity constraints in optimization formulations. We evaluate CIRNO by implementing three recent works on optimization. We demonstrate the relevance of CIR and CIRNO in DNs/UDNs through a significant reduction in convergence times (by over 50%) while maintaining high accuracy (over 95%). To the best of our knowledge, this is the first work to statistically analyze CIR in DNs/UDNs and LTE-WiFi heterogeneous networks (HetNets) and to use CIR regression equations in network optimization. © 2020 IEEE.