Rutile pigment with preadsorbed monomers of acrylamide (AM) or acrylic acid (AA) has been treated in air corona discharges at various input power levels for times from 30-120 s. Inverse gas chromatographic data showed that the treatments reduced dispersive surface energies and significantly altered the acid/base interaction potential of the surfaces. Inferred is the corona-activated synthesis of oligomeric or polymeric structures anchored to the pigment surface. XPS analyses report modifications in the chemical structure of pigment surfaces, which are consistent with the suggested consequence of corona treatment. When incorporated into LLDPE and PVC host polymers, compounds with the corona-modified rutiles have better mechanical properties than analogues with untreated pigment, notable being improved elastic moduli, yield stresses, and stress/strain relationships at break. AM-modified rutiles were preferable to AA-modified versions in this regard. The addition of treated pigments to immiscible LLDPE/PVC (75/25) blends resulted in similar benefits to mechanical properties, AM pretreatment again being preferred. Stronger acid-base interaction at contacts between corona-modified rutiles and the PVC component is an apparent reason for improved mechanical properties. Speculatively also, AM pretreatments lead to attached chains of sufficient length to entangle with the LLDPE, further strengthening the interphase and relevant bulk properties.