The Herbert E. Valentine Papers includes scrapbooks, diaries, correspondence, sketches, photographs, printer's blocks, newspaper clippings, and books created by Valentine both during and after the Civil War. The material has been arranged chronologically to reflect Valentine's creative approach. Diary extracts, letters, sketches, and a sketchbook document Valentine's military service with the 23rd Regiment Massachusetts Volunteer Infantry during the Civil War. Valentine's personal copy of James Emmerton's publication on the 23rd Regiment includes multiple annotations and sketches added by Valentine. The scrapbook in Box 3 was created by Valentine himself and contains newspaper clippings of veteran affairs; due to preservation concerns, correspondence has been removed from the scrapbook and rehoused in folders, located within Box 3. These letters remain in the order they appeared within the scrapbook. Valentine's personal copy of his publication Story of Co. F., includes additional handwritten notes, photographs, sketches, and appendices. Printer's blocks used in the creation of the book are included in this collection as well.

Valentine's personal involvement with veteran organizations is reflected in his publication 101 Brush Drawings in Sepia & Neutral Tint from Sketches made during the Civil War 1861-1864, a publication based on his earlier sketchbook and dedicated to his fellow members of Company F. Valentine also created a scrapbook to commemorate the dedication of the monument erected in the National Cemetery in New Berne, North Carolina in honor of those soldiers from Massachusetts who fought and died in the Civil War. Finally, from 1911 until 1915, Valentine created nine volumes entitled "War Day by Day" that include clippings from the Salem Gazette and Boston Daily Advertiser, documenting significant Civil War moments.