Tumor theranostics (a portmanteau of therapeutics and diagnostics) is now achieved in various ways with complex nanoparticle systems. Layered double hydroxide (LDH) nanoparticles are effective at drug/gene delivery and as imaging agents in potential tumor theranostics. This mini-review paper summarizes recent progress in developing LDH nanoparticles as a pH-sensitive magnetic resonance imaging (MRI) contrast agent, as a positron emission tomography (PET) imaging agent, and as a co-delivery platform for two therapeutic agents for tumor diagnosis and therapy. These results have indicated clearly the potential application of LDH nanoparticles for simultaneous diagnosis and treatment of cancers.