Tobacco (Nicotiana tabacum L.) is a major industrial crop that has being cultivated for centuries for the manufacturing of cigarettes, cigars, and other smoking products. Due to its negative effects on both human health and the environment, the European Union has adopted strict policies that aspire to reduce the consumption of tobacco. Herbal cigarettes are alternative smoking products that are often advertised as healthier than conventional tobacco cigarettes and are especially popular in Asian markets. Even though the available literature suggests that they are equally detrimental to human health, the introduction of tobacco-alternative crops (TACs) to the European tobacco industry could smoothen the abandonment of tobacco, and eventually smoking products altogether, in the EU. The aim of the present systematic review was to compile a list of possible TACs that could be incorporated in the European smoking industry, and highlight their strengths and weaknesses. The most dominant crops in the literature (and in the existing market products) were calendula (Calendula officinalis L.), mullein (Verbascum thapsus L.), ginseng (Panax ginseng C.A.Mey.), tea (Camellia sinensis (L.) Kuntze), chamomile (Matricaria chamomilla L.), and mentha (Mentha spp.). Even though these crops are promising, further research is required for their incorporation in the European tobacco industry.