What writing materials did the writers of the Gospels use?

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We do not have any of the original manuscripts of the scriptures, nor any other evidence of what kind of materials were used. Presumably it would be the usual materials. The materials used have no theological significance.

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Echoing @djclayworth:

We do not have any of the original manuscripts of the scriptures, nor any other evidence of what kind of materials were used. Presumably it would be the usual materials.

Looking at other documents from around the same time period we can assume papyri and/or parchment (Dead Sea Scrolls).

2 John 1:12-3 or 3 John 1: 13 mentions that paper and ink were used during the time period by at least one of the apostles.

Having many things to write unto you, I would not write with paper and ink: but I trust to come unto you, and speak face to face, that our joy may be full.

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Jeremiah 22:14 states

Who says, "I will build myself a roomy house with spacious upper rooms, and cut out it's windows, paneling it with cedar and painting it bright red [vermillion]."

In terms of the ink, clearly certain dyes were available by the first century. In theory, the Hebrew Torah is produced the same way today as it was 3000 years ago. The type of ink would have been well known and common. The ink is a charcoal, water, and gum conglomeration; although they were not adverse to using animal blood. Charcoal inks were cheap, easy to obtain, and came out looking like black printer ink.

As for the paper, papyrus was common in Greece, but these were Jews from the Promised Land. They presumably waited long enough to be fluent in Greek before writing the Gospels, so they might have taken Greek customs as well. However, Jews were partial to animal skin parchment scrolls for long documents or codex--a parchment, papyrus hybrid--for shorter ones.

Rice paper, "paper," from the Far East did not make it to the West until the third century AD or so.

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