What concept related to the propellant mass contributes heavily to Starship's title as the "biggest"?

Answer

The propellant is the primary mass fraction that must be brought back and reused

The immense volume dedicated to propellant in both stages is critical because that propellant mass is the primary fraction that must be retained and reused, not discarded.

What concept related to the propellant mass contributes heavily to Starship's title as the "biggest"?

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