The move by the four Arab governments came despite mounting international pressure to compromise in their weeks-old boycott of their fellow US ally.
Saudi Arabia, the United Arab Emirates, Bahrain and Egypt blacklisted nine charity and media organisations and nine individuals "directly or indirectly linked to Qatari authorities" as "terrorist", a joint statement carried by the Saudi Press Agency said.
"We expect Qatari authorities to take the next step and prosecute the terrorist groups and people," the statement added.
The four governments have been boycotting Qatar since June 5 in the region's worst diplomatic crisis in years.
They sealed the emirate's only land border, ordered its citizens to leave and closed their airspace and waters to Qatari flights and shipping.
They demanded that Qatar break its longstanding ties with the Muslim Brotherhood, blacklisted as a "terror group" by the four governments although not by the international community.
They also demanded that it close broadcasting giant Al-Jazeera and a Turkish military base, and fall in line with Saudi-led policy in the region, particularly towards Iran.
Qatar has dismissed the demands as a violation of its sovereignty and has received significant support from its ally Turkey.
The four governments on Tuesday blacklisted three organisations based in Yemen and six based in Libya accusing them of ties to Al-Qaeda.
They also blacklisted three Qataris, three Yemenis, two Libyans and a Kuwaiti they said were implicated in "fundraising campaigns to support (former Al-Qaeda affilate) Al-Nusra Front and other terrorist militias in Syria".
Qatar and its neighbours support opposing sides in the conflict in Libya between a UN-backed unity government in Tripoli and a rival administration in the east.
Qatar supports Islamist militia that back the unity government, while the United Arab Emirates has provided arms deliveries to its rival that a UN panel found were in violation of UN sanctions.
Saudi Arabia has led a military intervention against Shiite rebels in neighbouring Yemen since March 2015.
Terrorists of both Al-Qaeda and ISIS have since expanded their presence in areas of the south under the nominal control of the Saudi-backed government.