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(1) Background: <i>Arthrospira</i> (commonly known as Spirulina) is an edible cyanobacterium that is produced worldwide as a food supplement owing to its high nutritional value. <i>Arthrospira</i> displays strong potential as an important ingredient in the development of novel functional foods. Polysaccharides from <i>Arthrospira</i> are biologically active compounds and hence there is interest in producing biomass rich in carbohydrates. (2) Methods: <i>A. platensis</i> was cultivated under different degrees of phosphorus limitation in order to trigger the accumulation of carbohydrates. The biomass was then characterized in terms of its content of α- and β-glucans, total dietary fiber and monosaccharide profile. Fourier-transform infrared spectroscopy (FTIR) was used for the rapid analysis of the main biomass components. (3) Results: Phosphorus limitation resulted in an increase in carbohydrates (from 23% up to 65% dry biomass) of which 4–12% (in relation to the dry biomass) was α-glucans and 20–34% was 1.3:1.6 β-glucans, while 1.4:1.6 β-glucans were not detected. Total dietary fibers ranged from 20–32% (of dry biomass), whereas among the carbohydrates, the predominant monosaccharide was glucose (>95%). FTIR performed well when applied as a prediction tool for the main biomass components. (4) Conclusions: Since β-glucans are of particular interest as biologically active compounds, this study demonstrates that phosphorus-limited <i>A. platensis</i> could be a potential ingredient for the development of novel functional foods.