The present work was carried out to obtain and highlight the fifth comprehensive baseline dataset on atmospheric deposition of trace elements and to assess air quality in Macedonia. In the period from August to September 2020, a total of 72 moss samples were collected in accessible areas in the country. The content of 28 elements (Ag, Al, B, Ba, Ca, Cd, Co, Cr, Cu, Fe, Ga, Hg, K, La, Mg, Mn, Mo, Na, Ni, P, Pb, S, Sb, Sc, Sr, Ti, U, and Zn) was determined using inductively coupled plasma–mass spectrometry. Based on the data obtained on the content of the elements, a factor analysis was carried out to identify and characterise different sources of pollution. In addition, distribution maps were created for all elements to show the regions most affected by anthropogenic activities. The survey conducted in 2020 has shown that air pollution with potentially toxic elements (PTEs) has slightly decreased compared to the results of the previous survey from 2015. This is due to the fact that, despite the operation of all mining and smelting facilities with the same capacity, government regulations for the installation of cleaning systems and additional regulations to reduce pollution have been introduced in the last five years. Nevertheless, the fact remains that the highest anthropogenic air pollution with PTEs is still caused by the operation of the ferronickel smelter in Kavadarci (Ni and Cr) in the southern part and by the lead and zinc mines in Probištip, Makedonska Kamenica, and Kriva Palanka in the eastern part of the country (Cd, Pb, and Zn).