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Abstract Conjugated polyelectrolytes (CPEs) exhibit a strong interplay between ionic and electronic properties, enabling tunable photophysical properties and charge transport dynamics. Polyelectrolyte complexation represents a versatile self‐assembly strategy to control the properties of CPEs by forming dense phases with varying optoelectronic and mechanical characteristics. This study focuses on ionically assembled complexes comprising oppositely charged self‐doped CPE (CPE‐K) and bottlebrush polyelectrolyte (BPE). It is demonstrated that subtle adjustments in the composition of CPE‐K:BPE blends enables tuning of photophysical and viscoelastic properties. It is observed that increasing the CPE‐K:BPE monomeric ratio from 1:1 to 1:3 in the initial solution for complexation induces a significant bathochromic shift in the maximum photoluminescence intensity of the dense phase, from 1.8 to 1.4 eV. Additionally, a higher BPE content enhances the softness and adhesion of the solid complex, while maintaining yield‐stress behavior and cyclability of the dense phase. The ability to electrochemically and statically dope the CPE‐K–BPE complex, effectively modulating its charge transport and optoelectronic properties is also demonstrated. This work underscores the potential of these complex‐fluid phases for developing soft, adhesive, and elastic mixed ionic‐electronic conductors with tunable properties for functional applications and 3D‐printing.