The potential use of nanoelectromechanical systems (NEMS) created in silicon nanopillars (SiNPLs) is investigated in this work as a new generation of aerosol nanoparticle (NP)-detecting device. The sensor structures are created and simulated using a finite element modeling (FEM) tool of COMSOL Multiphysics 4.3b to study the resonant characteristics and the sensitivity of the SiNPL for femtogram NP mass detection in 3-D structures. The SiNPL arrays use a piezoelectric stack for resonance excitation. To achieve an optimal structure and to investigate the etching effect on the fabricated resonators, SiNPLs with different designs of meshes, sidewall profiles, heights, and diameters are simulated and analyzed. To validate the FEM results, fabricated SiNPLs with a high aspect ratio of approximately 60 are used and characterized in resonant frequency measurements where their results agree well with those simulated by FEM. Furthermore, the deflection of a SiNPL can be enhanced by increasing the applied piezoactuator voltage. By depositing different NPs [i.e., gold (Au), silver (Ag), titanium dioxide (TiO2), silicon dioxide (SiO2), and carbon black NPs] on the SiNPLs, the decrease of the resonant frequency is clearly shown confirming their potential to be used as airborne NP mass sensor with femtogram resolution level. A coupling concept of the SiNPL arrays with piezoresistive cantilever resonator in terms of the mass loading effect is also studied concerning the possibility of obtaining electrical readout signal from the resonant sensors.