Despite a variety of T1-T2 dual-modal contrast agents (DMCAs) reported for magnetic resonance imaging (MRI), no tuning of local induced magnetic field strength of an DMCA, which is important to modulate the overall T1 and T2 responses for imaging delicate cells, tissues, and organs, is yet available. Here, we show that a spatial arrangement of T1 and T2 components within a "nano zone" in a single core-shell nanoparticle carrier (i.e., DMCA with core Fe3O4 and MnO clusters in a silica shell) to produce the necessary fine-tuning effect. It is demonstrated that this particle after the anti-CD133 antibody immobilization allows both T1 and T2 imaging at higher resolution for living ependynmal brain cells of rodents with no local damage under a strong MRI magnetic field. This study opens a route to rational engineering of DMCAs for accurate magnetic manipulations in a safe manner. Copyright © 2017 American Chemical Society.