An ensemble of nanosystems can be considered to improve magnetic resonance imaging (MRI) transverse relaxivity. Herein, an interacting superparamagnetic competing structure of an isotropic−anisotropic trimagnetic hybrid nanosystem, γ-Fe 2 O 3 @δ-MnO 2 @NiFe 2 O 4 , is considered for MRI relaxivity exploration. The interacting superparamagnetic system reveals fascinating dynamic magnetic behavior, where flower-shaped two-dimensional flakes are decorated over nanoparticles. The hybrid nanosystem exhibits modulated shape anisotropy with spin blocking and energy barrier broadening, which help in achieving faster MR transverse relaxivity. The hierarchical architecture ensemble of the trimagnetic landscape shows effective MR transverse relaxivity with a transverse (r 2 )/ longitudinal (r 1 ) relaxivity of 61.5 and potential cell viability. The competing trimagnetic system with regulated activation energy is found to be the underlying reason for such signal enhancement in MRI contrast efficiency. Hence, this study displays a novel pathway correlating MR transverse relaxivity with dynamic magnetic behavior and competing landscape of hierarchical trimagnetic ensembles.