In this work, scientific and systematic analysis was conducted for finding out the methods and techniques of ancient ink stick making. Analysis the ancient ink stick on ancient documents and wooden writing as letter or painting, we concluded as followings. From the analysis of ancient wood by dendrochronology, wood was cut at 1899, which provided the information on the year of ink stick's made on writing on ancient wood. Single particle size for soot of ancient ink stick was 107 nm for ink on the roof-filling timber in Sinsunwonjeon of Changdeok Palace, compared to 38 to 86 nm on the letter on ancient 12 paper document. Aggregate particle size was 370 nm for ink on the roof-filling timber in Sinsunwonjeon of Changdeok Palace, but 206 to 318 nm for aggregate particle size on 12 paper documents. There was similar pattern between single particle size and aggregate particle size of soot, which might provide the information of raw material for ancient ink. From infra-red and Raman spectroscopic analysis of sheet of writing on paper or wood, there was severe interference from background material (paper or wood). From Raman spectroscopic analysis of ancient ink carefully separated from ancient wood, spectrum pattern was closer to ink stick made by the soot from pine burning.