Polycyclic aromatic hydrocarbons (PAHs), PANHs, and peptoids dust spectral calculations from the interstellar medium (ISM) are important for dust observations and theory. Our goal is to calculate the radiation spectrum of spherical PAHs dust clusters in a vacuum containing ionized and applied in the presence of an electric field. We propose a new simple computational model to calculate the size of three-dimensional spherical dust clusters formed by different initial dust structures. By the Vienna Ab-initio Simulation Package code, the density functional theory with the generalized approximation was used to calculate the electron density gradient and obtain the radiation spectrum of dust. When the radius of spherical dust clusters is ∼[0.009–0.042] μm, the dust radiation spectrum agrees well with the Z = 0.02 mMMP stellar spectra, and the PAHs radiation spectrum of NGC 4676 at wavelengths of (0–5] μm and (5–10] μm, respectively. In the ionized state, the N-PAH, C10H9N, 2(C4H 4)1+, and peptoids 4(CHON), (C8H10N2O5)1+ dust clusters at 3.3 μm, while the 2(C22H21N3O 2)1+, 4(CHON) dust clusters at 5.2 μm have obvious peaks. There is a characteristic of part of PAHs and peptoids clusters radiation at the near-infrared wavelength of 2 μm. However, especially after applying an electric field to the dust, the emission spectrum of the dust increases significantly in the radiation wavelength range [3–10] μm. Consequently, the dust clusters of PAHs, PANHs, and peptoids of the radius size ∼[0.009–0.042] μm are likely to exist in the ISM.