<?xml version="1.0" encoding="UTF-8"?>

<!--XBRL Document Created with the Workiva Platform-->
<!--Copyright 2026 Workiva-->
<!--r:01a16ab5-7966-7706-b507-25b02d8d478e,g:fa944ec7-1f0f-4121-829c-34df3f5fa003-->
<link:linkbase xmlns:link="http://www.xbrl.org/2003/linkbase" xmlns:xlink="http://www.w3.org/1999/xlink" xmlns:xsi="http://www.w3.org/2001/XMLSchema-instance" xmlns:xbrldt="http://xbrl.org/2005/xbrldt" xsi:schemaLocation="http://www.xbrl.org/2003/linkbase http://www.xbrl.org/2003/xbrl-linkbase-2003-12-31.xsd">
  <link:arcroleRef arcroleURI="http://xbrl.org/int/dim/arcrole/all" xlink:type="simple" xlink:href="http://www.xbrl.org/2005/xbrldt-2005.xsd#all"/>
  <link:arcroleRef arcroleURI="http://xbrl.org/int/dim/arcrole/hypercube-dimension" xlink:type="simple" xlink:href="http://www.xbrl.org/2005/xbrldt-2005.xsd#hypercube-dimension"/>
  <link:arcroleRef arcroleURI="http://xbrl.org/int/dim/arcrole/dimension-default" xlink:type="simple" xlink:href="http://www.xbrl.org/2005/xbrldt-2005.xsd#dimension-default"/>
  <link:arcroleRef arcroleURI="http://xbrl.org/int/dim/arcrole/dimension-domain" xlink:type="simple" xlink:href="http://www.xbrl.org/2005/xbrldt-2005.xsd#dimension-domain"/>
  <link:arcroleRef arcroleURI="http://xbrl.org/int/dim/arcrole/domain-member" xlink:type="simple" xlink:href="http://www.xbrl.org/2005/xbrldt-2005.xsd#domain-member"/>
  <link:roleRef roleURI="http://gevo.com/role/DocumentandEntityInformation" xlink:type="simple" xlink:href="gevo-20261023.xsd#DocumentandEntityInformation"/>
  <link:definitionLink xlink:role="http://gevo.com/role/DocumentandEntityInformation" xlink:type="extended">
    <link:loc xlink:type="locator" xlink:label="loc_dei_EntityInformationLineItems_01a16aca-cc5a-7ab3-987e-f11423938c6c" xlink:href="https://xbrl.sec.gov/dei/2025/dei-2025.xsd#dei_EntityInformationLineItems"/>
    <link:loc xlink:type="locator" xlink:label="loc_dei_EntitiesTable_01a16aca-cc59-73ae-9dfa-8d630b8826b9" xlink:href="https://xbrl.sec.gov/dei/2025/dei-2025.xsd#dei_EntitiesTable"/>
    <link:definitionArc xlink:arcrole="http://xbrl.org/int/dim/arcrole/all" xlink:from="loc_dei_EntityInformationLineItems_01a16aca-cc5a-7ab3-987e-f11423938c6c" xlink:to="loc_dei_EntitiesTable_01a16aca-cc59-73ae-9dfa-8d630b8826b9" xlink:type="arc" order="1" xbrldt:closed="true" xbrldt:contextElement="segment"/>
    <link:loc xlink:type="locator" xlink:label="loc_dei_DocumentPeriodEndDate_01a16aca-cc5a-70a8-b219-f0b9c0836dfc" xlink:href="https://xbrl.sec.gov/dei/2025/dei-2025.xsd#dei_DocumentPeriodEndDate"/>
    <link:definitionArc xlink:arcrole="http://xbrl.org/int/dim/arcrole/domain-member" xlink:from="loc_dei_EntityInformationLineItems_01a16aca-cc5a-7ab3-987e-f11423938c6c" xlink:to="loc_dei_DocumentPeriodEndDate_01a16aca-cc5a-70a8-b219-f0b9c0836dfc" xlink:type="arc" order="0"/>
  </link:definitionLink>
</link:linkbase>