Magnetic hyperthermia and magnetic resonance imaging (MRI) are two of the most important biomedical applications of magnetic nanoparticles (MNPs). However, the design of MNPs with good heating performance for hyperthermia and dual T1/T2 contrast for MRI remains a considerable challenge. In this work, ultrasmall superparamagnetic iron oxide nanoparticles (USPIONs) are synthesized through a simple one-step methodology. A post-synthetic purification strategy has been implemented in order to separate discrete nanoparticles from aggregates and unstable nanoparticles, leading to USPIONs that preserve chemical and colloidal stability for extended periods of time. The optimized nanoparticles exhibit high saturation magnetization and show good heating efficiency in magnetic hyperthermia experiments. Remarkably, the evaluation of the USPIONs as MRI contrast agents revealed that the nanoparticles are also able to provide significant dual T1/T2 signal enhancement. These promising results demonstrate that USPIONs are excellent candidates for the development of theranostic nanodevices with potential application in both hyperthermia and dual T1/T2 MR imaging.