This article describes the preparation and fundamental properties of a new possible material as a magnetic resonance imaging contrast agent based on the incorporation of preformed iron oxide (Fe
3
O
4
) nanocrystals into hollow silicon nanotubes (Si NTs). Specifically, superparamagnetic Fe
3
O
4
nanoparticles of two different average sizes (5 nm and 8 nm) were loaded into Si NTs of two different shell thicknesses (40 nm and 70 nm). To achieve proper aqueous solubility, the NTs were functionalized with an outer polyethylene glycol-diacid (600) moiety via an aminopropyl linkage. Relaxometry parameters
r
1
and
r
2
were measured, with the corresponding
r
2
/
r
1
ratios in phosphate buffered saline confirming the expected negative contrast agent behaviour for these materials. For a given nanocrystal size, the observed
r
2
values are found to be inversely proportional to NT wall thickness, thereby demonstrating the role of nanostructured silicon template on associated relaxometry properties.