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The self-assembly of block polymers into well-ordered nanostructures underpins their utility across fundamental and applied polymer science, yet only a handful of equilibrium morphologies are known with the simplest AB-type materials. Here, we report the discovery of the A15 sphere phase in single-component diblock copolymer melts comprising poly(dodecyl acrylate)− block −poly(lactide). A systematic exploration of phase space revealed that A15 forms across a substantial range of minority lactide block volume fractions ( f L = 0.25 − 0.33) situated between the σ-sphere phase and hexagonally close-packed cylinders. Self-consistent field theory rationalizes the thermodynamic stability of A15 as a consequence of extreme conformational asymmetry. The experimentally observed A15−disorder phase transition is not captured using mean-field approximations but instead arises due to composition fluctuations as evidenced by fully fluctuating field-theoretic simulations. This combination of experiments and field-theoretic simulations provides rational design rules that can be used to generate unique, polymer-based mesophases through self-assembly. 

Polymer blending is a cost‐effective way to control the properties of soft materials, but the propensity for blends to macrophase separate motivates the development of efficient compatibilization strategies. Across this broad area, compatibilization is particularly important for polysiloxanes, which exhibit strong repulsive interactions with most organic polymers. This review analyzes state‐of‐the‐art polysiloxane compatibilization strategies for silicone–organic polymer blends. Emphasis is placed on chemical innovation in the design of compatibilization agents that may expedite the commercialization of new silicone–organic materials. We anticipate that hybrid silicone blends will continue to play an important role in fundamental and applied materials science across industry and academia.