A nanocapsule shell of poly(ethylene glycol)-block-poly(d,l-lactic acid) (PEG-b-PLA)
mixed with anionic Eudragit S100 (90/10% w/w) was previously used
to entrap and define the self-assembly of indigo carmine (IC) within
the hydrophilic cavity core. In the present work, binary blends were
prepared by solution mixing at different PEG-b-PLA/Eudragit
S100 ratios (namely, 100/0, 90/10, 75/25, and 50/50% w/w) to elucidate
the role of the capsule shell in tuning the encapsulation of the anionic
dye (i.e., IC). The results showed that the higher content of Eudragit
S100 in the blend decreases the miscibility of the two polymers due
to weak intermolecular interactions between PEG-b-PLA and Eudragit S100. Moreover, with an increase in the amount
of Eudragit S100, a higher thermal stability was observed related
to the mobility restriction of PEG-b-PLA chains imposed
by Eudragit S100. Formulations containing 10 and 25% Eudragit S100
exhibited an optimal interplay of properties between the negative
surface charge and the miscibility of the polymer blend. Therefore,
the anionic character of the encapsulating agent provides sufficient
accumulation of IC molecules in the nanocapsule core, leading to dye
aggregates following the self-assembly. At the same time, the blending
of the two polymers tunes the IC release properties in the initial
stage, achieving slow and controlled release. These findings give
important insights into the rational design of polymeric nanosystems
containing organic dyes for biomedical applications.