The antimicrobial properties of bagasse paper sheets coated with natural polymers (chitosan, different ratios of (gelatin/glycerol) + chitosan, hemicellulose, hemicellulose + glycerol, hemicellulose+chitosan) or synthetic organophosphorus dimer compounds were evaluated in this work. Hemicelluloses showed moderate activity against Bacillus subtilis and Candida albicans, while chitosan showed weak activity against B. subtilis. The condition that offered the highest inhibitory activity of bagasse paper was the one coated with 1,3-diaryl-2,2,2,4,4,4 hexachlorocyclodiphosph(V)azane (where aryl is p-chloroaniline or p-anisidine). The developed bagasse papers were evaluated against Gram-positive bacteria, Gram-negative bacteria, yeasts, and fungi. The highest inhibitory activity was obtained at a concentration of 200 mg/mL for p-chloroaniline with an inhibition zone that varied for different microbes from 6.9 mm to 26 mm. The highest inhibitory activity was obtained at 300–250 mg/mL for p-anisidine against most of the pathogenic microorganisms with an inhibition zone that varied for different microbes from 8 mm to 14.75 mm. The observed antimicrobial and antifungal activity properties for bagasse paper coated with 1,3-diaryl 2,2,2,4,4,4-hexachlorocyclodiphosph(V)azane could be attributed to the presence of Cl, P atoms, and the lone pair of electrons on N atoms in the structure of the dimers.