Pine needles from various species have long been utilized as bioindicators of air pollution. The accumulation of major and trace elements in these needles results from both dry and wet deposition of airborne pollutants, as well as the uptake of substances through plant roots. Environmental pollutants can be transported over long distances and reach remote areas. To investigate this, a mountainous region at the confluence of the Lower Inn Valley and Achental in Tyrol, Austria, was selected for sampling. Needles from mountain pines (Pinus mugo) were collected at three different sites at altitudes from 1400 meters to 2000 meters. Sampling covered needles of varying ages—young, one-year-old, two-year-old, and older—from five to ten trees at each site, pooling needles of the same age. Sampling was conducted annually every July from 2018 to 2024. For elemental analysis, dried samples underwent acidic digestion (either microwave assisted or by high pressure asher) followed by quadrupole and high-resolution inductively coupled plasma mass spectrometry (ICP-MS) measurements. The metabolic state of the plant material was monitored in a fast and non-destructive way by Raman spectroscopy providing additional information on the growing conditions of the mountain pines. The highly sensitive differentiation in fingerprint region of the spectra allows the classification of differently grown pine needles. Rigorous quality assurance protocols were implemented to ensure the reliability of the analytical results and their comparability with previously published data. The findings revealed that altitude had a greater effect on the concentrations of macroelements than on potentially toxic elements. Like other pine species, age-related accumulation of certain elements was observed in the needles.