Polypeptide secondary structure controls the dimensions of aggregates formed from a polybutadieneb-poly(L-glutamic acid) diblock copolymer after direct dissolution into water. The hydrodynamic radius (RH) of these aggregates (even at high NaCl concentrations) were found to correlate (see picture) with a transition from a compactly folded α-helical poly(L-glutamic acid) block at low pH to an extended random coil conformation at basic pH.