The chamomile drug (Chamomillae anthodium) is widely known and has been used as a medicine for ages. Today, the drug is officially registered in the European Pharmacopoeia. Despite the economic importance of the chamomile Matricaria recutita L., little is known about the extent and nature of the essential oil variability and composition of this species in Albania. Therefore, information about the extent of the uses of various gene pools is extremely valuable for the development of future chamomile cultivation and breeding programs. This study aimed to analyze the differences among 29 populations in different sites in central Albania. The quantities of essential oils ranged from a low of 0.10 ± 0.01% in Fier and Tirana to a high of 0.75 ± 0.05% in Linzȅ. The yield of volatile oils depended on the geography, altitude, and other factors, including stress influences on the site of plant population growth. This fact was confirmed by various subclimatic characteristics obtained from individual localities. Essential oil extracted from chamomile inflorescences was recorded to have between 23 and 43 chemical components. It was found that /-/-α-bisabololoxides B and A were the major constituents in 25 samples, with only 4 having dominant /-/-α-bisabolol. The uniquely determined chemical type of the chamomile wild populations in Albania was chemical type B (/-/-α-bisabololoxide B > /-/-α-bisabololoxide A > /-/-α-bisabolol). Based on the study of chamomile’s pharmacodynamic properties, the sesquiterpenes /-/-α-bisabolol and chamazulene are considered to be the most valuable constituents. Consequently, a very intensive improvement breeding program must begin, with emphasis on drug yield, polyploidization, essential oil quantity, and both component contents in the oil.