The Langmuir-Schaefer (LS) technique was applied to prepare two-dimensional films of tridodecylamine (TDA)- stabilized Co nanoparticles. Ethylene glycol was used as the subphase because the Co nanoparticles spread better on it than on water. Surface pressure-area isotherms provided very little information on the floating films, and Brewster angle microscopy (BAM) was needed to characterize the film formation in situ. In addition to the subphase, various other experimental factors were tested in the LS filmpreparation, including solvent and presence of freeTDAligands and poly(styrene-b-ethylene oxide) (PS-b-PEO) in the nanoparticle dispersion. LS films deposited from dispersions fromwhich the excess TDAligands had been removed by washing the Co nanoparticles with 2-propanol consisted of hexagonally organized particles in rafts that were organized in necklace structures. The addition of PS-b-PEO to the deposition dispersion resulted in small nanoparticle rafts evenly distributed over the substrate surface. The best Co-nanoparticle-PS-b-PEO films were obtained with a mass ratio of 20:1 between Co (9 nm) and block copolymer (38 200 g/mol, PEO content 22 mass %). These films were successfully transferred onto Formvar-coated TEM grids and characterized by transmission electron microscopy (TEM) and a superconducting quantum interference device (SQUID) magnetometer. At room temperature the films showed superparamagnetic behavior with a saturationmagnetizationMs of 100 emu/g (Co). Our work indicates that it is possible to obtain thin superparamagnetic LS films of TDA-stabilized Co nanoparticles. This is an important result as the TDA-stabilized Co nanoparticles show a very good resistance to corrosion.