Understanding the influence of surface roughness on the deposition of nanoparticles is important to a variety of environmental and industrial processes. In this work, slanted columnar thin films (SCTFs) were engineered to serve as an analogue for rough surfaces with controlled height and surface properties. The deposition of titanium dioxide nanoparticles (TiO(2)NPs) onto alumina-or silica-coated SCTFs (Al2O3-Si-SCTF, SiO2-Si-SCTF) with varying heights (50 nm, 100 nm, and 200 nm) was measured using a combined quartz crystal microbalance with dissipation monitoring (QCM-D) and generalized ellipsometry (GE) technique. No TiO2NP deposition was observed on flat, silica-coated QCM-D sensors or rough, 100 nm thick SiO2-Si-SCTF. TiO2NP deposition onto Al2O3-Si-SCTFs in ultra-pure water was significantly higher than on the flat alumina-coated QCM-D sensor, and deposition increased as the roughness height increased. The nanoparticle attachment was sensitive to the local flow field and the interaction energy between nanoparticles and the QCM-D sensor. At a higher ionic strength condition (100 mM NaCl), TiO2NP aggregates with varying sizes formed a rigid layer on top of SCTFs. For the first time, deposition of nanoparticles was measured as a function of roughness height, and the impact of roughness on the properties of the attached nanoparticle layers was revealed. This finding indicates that key parameters describing surface roughness should be explicitly included into models to accurately predict the transport of nanoparticles in the subsurface.