The interplay of the isotropic–nematic transition and phase separation in lyotropic solutions of two types of semiflexible macromolecules with pronounced difference in chain stiffness is studied by Density Functional Theory and Molecular Dynamics simulations. While the width of the isotropic–nematic two-phase coexistence region is narrow for solutions with a single type of semiflexible chain, the two-phase coexistence region widens for solutions containing two types of chains with rather disparate stiffness. In the nematic phase, both types of chains contribute to the nematic order, with intermediate values of the order parameter compared to the corresponding single component solutions. As the difference in bending stiffness is increased, the two chain types separate into two coexisting nematic phases. The phase behavior is rationalized by considering the chemical potentials of the two components and the Gibbs excess free energy. The geometric properties of the chain conformations under the various conditions are also discussed.
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